In The Secret Of Mamo, Lupin manages to drive on a road's guard rail, which at the time was suspended in mid-air, and safely makes it back onto the road. Ridiculous? Yes. Awesome? Definitely.
Speaking of car chases, the entire opening car chase in The Castle of Cagliostro. Lupin manages, among other feats, to drive up a vertical cliff-face to rescue a mysterious girl.
Long-standing anime folklore has it that Steven Spielberg himself has pronounced this scene as the best car chase ever put on film.
The manga chapter The Great Escape has Lupin spending a year in prison claiming that he's not really Lupin. When the time comes for his execution, he switches places with one of the guards. The guard naturally starts screaming that he's not really Lupin, but no-one believes him after what Lupin's been doing. Once Zenigata finds out, he races down the hall screaming to stop the execution as Lupin walks calmly out of the prison, smiling. He spent an entire year in prison just to humiliate Zenigata to the same degree that the Inspector managed against Lupin a year prior.
Along with a huge Crowning Moment of Heartwarming, the second series episode "Goemon's Close Call" also has an epic moment towards the end. Goemon is given a chance to avenge himself against one of the assassins who tortured him throughout the episode; his hands, however, have practically been mangled by what he's been through. He charges forth anyway, Zantetsuken tucked under one arm, and manages draw and run through his foe anyway... by grabbing the sword with his teeth.
Another moment for Goemon in the episode "The Rose and the Pistol", where's he's spent the whole episode being hungry since he can't find real Japanese food in Spain. He refuses to go along with Lupin to his challenge with the villain of the episode since Lupin lied about a "real Japanese restaurant" being in Barcelona... and just to emphasize that he takes his food seriously, Goemon silently faces the night sky and cuts a shooting star in half. Lupin's so dumbfounded that he turns to the viewer and says "No way! Impossible!"
Whenever Zenigata gets serious, he's prone to pulling off these - just mainly when his aim isn't to put Lupin behind bars even if he's the target. Once he managed to outwit and handcuff all three of the gang to a tree, just because he wanted to warn them about specialist hitmen they'd be going up against.
This appears to be based on a scene in the manga where Zenigata manages to defeat both Jigen and Goemon by outmaneuvering them then handcuffing them to a tree. The best part is Lupin looking at the reader and asking "Can you believe this shit?!"
He also manages to catch the three again when he wants to steal back some family heirlooms.
"The Buried Treasure of Genghis Khan" has him easily figuring out Lupin's plan to steal the Khan family treasure and actually managing to trick Lupin into walking straight into his police car. Lupin only manages to escape by using dynamite.
The ending of The Secret of Mamo has Lupin outsmarting a billion-year-old psychic brain in a jar that called itself god.
The ending of The Gold of Babylon has Lupin stealing the golden tower of Babel from aliens who were called God by humans.
In the Elusiveness of Fog, Lupin tricks Mamou, a guy who invented a time-travel machine, into letting him steal the device. He does the same thing in the manga and the first series episode based on said chapter of the manga. It also overlaps with Crowning Moment of Funny.
The final (numbered) chapter of the first manga series. Throughout the chapter, a timer is counting down at the bottom of each panel. Zenigata has Lupin and co. surrounded in a field. Lupin whips out a sheet and throws it over them. Zenigata yanks the sheet off only to find that Lupin has used some sleight-of-hand to replace himself, Jigen, and Goemon with a group of astronauts. One of them mentions that it's too late for Zenigata to catch them. Cut to the timer running out as, in a rare two-page spread, a nearby space shuttle launches, implying Lupin escaped to space leaving behind a (moreso than usual) dumbfounded Zenigata.
In a second series episode, Zenigata was in Israel when he found out that Lupin was in Egypt, and got arrested because he demanded a plane ticket for a country that Israel was at war against. Later in the episode, Lupin's gang is in the desert... And we find out that Zenigata got his ticket and command of the whole Egyptian police after coming straight from Israel.
Lupin's animation history has had his saga feature the best in Japanese animation: Hayao Miyazaki, Osamu Dezaki, Gisaburo Sugii, Hiroyuki Imaishi, Takeshi Koike and many others all contributed to working on a Lupin III feature, featuring their own distinct animation styles/trademarks.
Daisuke Jigen's voice actor Kiyoshi Kobayashi has voiced the role from the very first animated Lupin feature. As of 2019, it's 52 years.