Crime boss Rupert Thorne was a recurring villain, and was overweight.
One episode had Bruce Wayne, with amnesia, kidnapped and forced to work in a mining camp by Boss Biggis, a white-suited obese man who was always munching on a turkey leg. When one of the man's henchmen tried to remind him that the exhausted slaves have to eat, he replied, "I have to eat. They have to work."
Harvey Bullock is a downplayed example. He's repeatedly shown to be rude, filthy, in love with donuts and a general mess, but he's an honest cop and just as dedicated to taking down criminals as Commissioner Gordon and Batman, even if he butts heads with Batman.
The Batman gives us the overweight, incompetent, self-righteous Chief Rojas, a man who thinks what he says goes and helped to ruin the life of one of his officers, Ethan Bennett, just because Bennett supported Batman. Also, Dr. Hugo Strange is obese (and rather ugly) in this version.
Lawrence Limburger from the original series. It's implied obesity is a sign of high rank in Plutarkians (being Planet Looters who strip other planets bare for natural resources), with most of the seen Plutarkians being very bloated (Limburger's sister even mentions going to the Plutarkian "fat farm" and wanting to get there before all the good fat is gone). The only skinny Plutarkians seen are Marshal (Limburger's pre-teen hellion of a nephew), One-Eyed Jack Monterey (a Plutarkian agent stationed in Las Vegas), Gutama Gouda (a Plutarkian agent stationed in Los Angeles), Dominic T. Stilton (Limburger's former superior from the episode "Once Upon a Time on Mars") and a lawyer named Perry Provolone.
The 2006 revival has one of the major villains being a Corrupt Corporate Executive named Ronaldo Rump, who is mainly fat because, as his name implies, he has a huge rear end.
The Boondocks has several overweight characters, and most of them are unpleasant.
In Codename: Kids Next Door, there is the overweight Shogun Roquefort, the Cheese Shogun. However, despite being a bastard (he blackmails restaurants into giving them their cheese and forces both kids and adults alike to work as slave labor in his cheese mines) he's really not a very competent villain at all. His Mooks are competant fighters, while he knocks himself out by hitting his head on the ceiling when confronting Numbuh Two.
Toot from Drawn Together, who is overweight and bitter about it. She's shown to eat people, and to consume too much food. Becomes more sympathetic later.
So overweight, in fact, that at one point it takes her nervous system about two minutes to relay pain to her brain. Said pain was a sword Xandir stabbed into her back as a bet.
There was also an episode where she ended up on an island as a beached whale.
In Family Guy, Peter Griffin's tendency to invoke this trope is probably the most obvious difference between him and Homer Simpson. While Homer can gobble down platefuls of food for laughs, Peter's usually only shown in the same context as food when the point is supposed to be that he's a Jerkass.
One episode in particular stands out - Peter forms an awareness group for fat people discrimination, and every last one of them conforms to this trope, making disturbing groaning noises, busting out snacks every few minutes, and making excuses for all their actions. One half-dead fat guy actually interrupts the action to ask if he can eat a dead fat guy that's in the same room as he is.
In a cutaway scene from the episode Brian Sings and Swings, John Goodman is portrayed as this.
Peter actually has a repressed fat-fetish.
...which brings us to the other standout episode of this trope: When Peter gets a vasectomy and loses all interest in Lois, she starts pigging out, and he starts to make jokes about her weight...until said fat fetish busts out and breaks the bed.
Only averted sometimes by Chris Griffin and averted always with Cleveland (now a protagonist all his own), and Cleveland Jr., who are all fat but are also among the show's few genuinely decent tempered characters. Chris is with his dad in the Fat Idiot trope though, but he's still far less vicious generally. Cleveland is rather intelligent.
When Chris in one episode makes an attempt to lose weight, Stewie taunts and mocks him relentlessly. As the episode goes on, Stewie pigs out and eats more and more to taunt Chris with the food he cannot eat. This causes Stewie to gain lots of weight over time and as he gets bigger, he becomes more of a slob (he slams his face into a chocolate cake and eats like a pig), his girth breaks his high chair, and he grows so lazy to the point where his insults are lazily made and he falls asleep in the middle of it before he can finish his ice cream.
The protagonist of the animated short La Faim. While he is not a particularly nasty person, he disgusts the audience due to his complete and utter selfishness; he cares about absolutely nothing in life outside of his own pleasures. His gluttonous gorging gets more and more over-the-top as the short goes on (facing a full banquet table, he becomes an Eldritch Abomination made of mouths and arms so he can eat it all, and then becomes a steamshovel as he devours the table itself), and he morphs from a handsome young man into a morbidly obese slug. Finally the short ends when the man realizes the cost of his lifestyle: millions of children across the world are starving. He is surrounded by starving waifs, who proceed to...well, you can probably guess from here.
In the My Little Pony: Friendship Is Magic episode "Inspiration Manifestation", Rarity is commissioned to build a puppet show theater for an overweight puppeteer. He brutally criticizes the work she did and his weight is Played for Laughs when he tries to squeeze into the theater.
InThe Smurfs there was Lord Balthazar, Gargamel's godfather, a more competent, far crueler wizard, who was overweigh. Something of an Upper-Class Twit, it was suggested he had fondness for rich foods.
The Oblongs gives us Helga, a rude, ugly, mobidly obese little girl with delusions of grandeur. At least, they connect it to being underprivileged (she can only affored to eat thrown out wedding cakes, she lives next to an abandoned factory...) And she is still awesome!
Pete in all of his roles in Disney stuff is incredibly fat and an incredible bastard. The degrees of bastardy have varied over the years, but he always qualifies. Averted with his son P.J., in Goof Troop, who's shaped like him (but with less of the ugly) and is a really nice kid.
Miss Finster, Gellman, and Kurst the Worst in Recess.
There's also Koreo, a thuggish fifth grader who hangs around Lawson.
Mr. E in Scooby-Doo! Mystery Incorporated. He was much skinnier as a teenager and is in shape in the new timeline, in which he's very Steve Jobs-esque. This makes sense, considering he's actually Ricky Owens, who's clearly meant to be Shaggy's analogue in the original Mystery Incorporated. The adult Mr. E gives us an idea of what Shaggy would look like if his famous love of junk food ever caught up with his physique.
Homer, despite what one may initially think, mostly averts this trope. When 75% of the entire cast is fat - Springfield is the fattest city in America! - the fat people come in all temperaments. Everyone who's fat has their Fat Bastard moments, but it isn't always consistent, especially with the Negative Continuity.
There are near-consistent straight cases, though, even if the fat and the bastardy aren't directly related. Mayor Quimby's girth could be taken to represent him being one of the "fat cats" (a derogatory term for over-privileged and corrupt politicians). Jeff Albertson the Comic Book Guy is nasty and self-defeatingly pompous, and is not above using profiteering to make money. Fat Tony belongs to an evil profession. Nelson is a big fat bully (though he does have some moments of decency, especially when he's interacting with Lisa).
Home can show it at times, like the episode where Homer selfishly and stupidly became horrendously obese just to be able to work at home and avoid 15 minutes of exercise a week. (But he did become the hero in the end.)
Slightly inverted in that the most actively evil characters on the show, Mr. Burns and Sideshow Bob, are thin.
One example of how this trope is zig-zagged in the show is the trio of bullies: Jimbo and Dolph are thin, while Kearney is fat.
Eric Cartman of South Park. Most notably in two episodes where 1), during his family reunion, all of his family members, save for his mother and grandmother who are thin and caring, are fat annoying slobs. 2) Where Eric from the future, who lost weight and became a better person in general (and wealthy to boot), came to the past to tell Eric to be a good human being. Eric (thinking it was a trick) delivered the generic "screw you" line and said he would stay the way he was, after the other characters were out of view the future Eric transformed into a dirty obese mechanic as a result of his younger self not "changing for the better".
Rob Reiner in the episode "Butt Out" uses propaganda to point out the dangers of smoking while ignoring his obesity to the point he needs butter to squeeze out of his limo.
Patrick occasionally shows traits of this, especially in later episodes thanks to Flanderization, "Rule Of Dumb" is a very extreme example where he goes mad with royal power.
Mr. Krabs may also count at times, though less emphasis is put on his rotund build for the most part.
Oleander, a zaftig villain from Sushi Pack, although she's only a villain because she's a foodee and wants to eat the Sushi Pack (who don't help things by describing themselves as "bite-sized bits of bravery" and "finger foods of freedom").
Krang from Teenage Mutant Ninja Turtles (1987) plays with this, and Stout Strength as his android body is an overweight looking humanoid, however the suit itself was never shown to be sentient, or evil in itself. The Ninja Turtles even made use of it at times.
Burne Thompson, the grumpy editor, and April's grouchy boss is portrayed as one in the toyline along with Fat Slob which exaggerates his overweight body by giving him an unbuttoned shirt, portrays him chewing with his mouth open, and holding a giant sandwich.
The 2003 cartoon: original villain Garbageman is a grotesquely obese man covered in food-stains, and drools who lives on a garbage island, and enslaves the homeless to be his subjects. Due to his weight, and having no legs, he rides around in a tank.
The 2012 Ninja Turtles: Vic was an overweight man in an undershirt who records the Ninja turtles for blackmail purposes, and is completely ungrateful when they rescue him. He gets turned into the mutant, Spiderbytez, a perfectly spherical Spider which shoots webs via farting, he blames the Turtles, and becomes a Super Villain.
Bebop wasn't fat in the 1987 version, but he clearly packed on the pounds in the updated 2012 one.
Three of the Gene Deitch-directed Tom and Jerry shorts gave Tom an owner who routinely beat the tar out of him when he screwed something up. It wasn't pretty.
Sugar from Total Drama. A cheating, manipulative and jerk fat girl that eat anything that remotely looks like food. She doesn't care who she hurts in order to win, especially Ella.