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Tear Jerker: The Smurfs
For the comics:
When the smurfs get tired of dealing with "The Smurfette", Jokey leads them in a vicious series of pranks that make her believe she's gained too much weight. The poor girl responds to this by nearly starving herself at dinner (while the others all talk about how GOOD it is and ask why she isn't eating), and is guilt-ridden about taking a single leaf — and after seeing herself in a trick mirror, she shuts herself away for days. And when Papa comes to check on her, he briefly fears she might have been Driven to Suicide. While she hasn't, she still cries that "I want to DIE!"
What makes this even worse is that this sort of thing also occurs in real life with far too many.
Smurfette: Oh, I'm so ashamed! I almost led you all to Gargamel's clutches, and you've been all so nice to me! Whatever you do to me, I deserve it. Throw me out of the village, abandon me in the forest, or send me back to Gargamel!
It doesn't help the fact that all of the Smurfs cried for that, even Grouchy who says "I hate sad!"
The sequel to this episode, "Smurfette Unmade" has this in spades where Gargamel has put her under a spell to turn her back to her original appearance with a malicious personality, something he should have done.
"Stop and Smurf the Roses," where Laconia the beautiful young wood elf is apparently killed after the evil Chlohydris kills all of the flowers (her life's source). When the Smurfs think that reversing her death-like state is irreversible, they tenderly lay her in a lilypad and prepare to lay her to rest ... until the moment of heartwarming comes when Papa Smurf is able to restore all the flowers to life.
Grandpa Smurf's apparent death in "Smurfquest".
The episode Squeaky, where Smurfette's pet mouse dies, and she runs away because she doesn't want to see her friends die.
The episode Clumsy Luck, when everyone believes Clumsy was crushed by a meteor. Even Papa Smurf is in tears.
Let's not forget Crying Smurfs, where Weepy Smurf is supposedly killed off. He's actually alive but the other Smurfs don't know this. Their reactions are heartbreaking.
Grouchy (of all smurfs) going out of his way to save Baby Smurf from being given back to the stork in "Once in a Blue Moon", running into the wilderness only to eventually end up returning to the village because keeping baby exposed to the elements would probably end up killing him. In spite of his hatred of everything, Grouchy had come to love Baby Smurf.
Grouchy: I hate giving up...
"Fire-Fighting Smurfs", where we see Snappy lamenting and crying over the damage done to the forest and animals. The guilt he feels tears your heart out so much.
For the 2011 movie:
When the Smurfs start feeling homesick and start missing the other Smurfs. Seeing poor Smurfette saying "Papa, do you really believe we'll get home to the other Smurfs?" is pretty sad, seeing her make puppy dog eyes doesn't help. Especially the fact they’re in a strange place.
Also, the scene where Papa Smurf tells the other Smurfs to save their lives, then Gargamel catches Papa Smurf with Smurfette yelling "Papa, No!" while Gutsy tells her "Keep moving lass, do as Papa says." and Smurfette saying "Papa" as they escape.