Him being able to do the artwork for the opening credits of Suburban Knights after various members of his family dying around that time.
The whole premise of the series is kinda this: find characters that are under-appreciated or forgotten and talk about what made them interesting or unique, often at great length and with considerable research. And in the process both introduce new fans to them, and give those who remember them a nice wave of nostalgia.
His review of The Batman episode of Babydoll with The Nostalgia Critic is, in itself a heartwarming moment, as CR nicely allowed NC to be a part of the review, & never once insulted the critic during that review, making him one of the few-or only- critic to do so.
The commentary is also quite nice. The two get along really well, and its nice to see them gush over a show they love so much, which they do a lot more now that they aren't trying to do a review.
At the end of the Big Daddy episode, he plays the song Butterfly Kisses to symbolize the relationship between Big Daddy and Hit Girl.
Just the fact that he still has the Tenderheart plushie that his grandmother gave him after he came home from the hospital.
Very brief moment in 12 More Forgotten Christmas Specials. In one scene, where a father is harshly berating his son, the video cuts to a picture of a sobbing Fluttershy. The image isn't what you'd call pleasant, but it's sweet to see CR make an unironic, if brief pony reference. A Christmas Miracle!
In the Daisy Head Mayzie review, while the end product didn't turn out all that well, he admits that there is the groundwork for a very good story, and even suggests it would make a good adaptation, given its obscurity. The episode in general has him gushing quite a bit over the work of Dr. Seuss.
His tribute to Marcia Wallace and Edna Krabappel for her performances that fleshed out teachers (yes teachers have a life outside the classroom and feelings) and for her Cancer Awareness works.
During the time of the Chilean earthquake, a fan approached him to thank him for his work and for giving him a little window to disconnect from the events unfolding around the earthquake. He is still in touch with that fan.