Anything in 4:3 (or close to it, like Academy) aspect ratio. I don't usually watch TV or movies (and especially not anime), so don't exclude anything just because you think it's too obvious. Don't worry about taste either, anything you think is worth watching is fine.

Starting off the thread with what I know (and can immediately think of):
IA has a ton of VHS rips e.g. https://archive.org/details/vhsvault

>Evangelion
Just finished the series, getting ready to watch the movie. A shame I waited this long to watch it.
Looks great on a CRT in a dark room.

>Cowboy Bebop
Haven't started yet.

>King of the Hill
Victim of seasonal rot. I don't remember where the cutoff is.

>Star Trek TNG / DS9
Required watching for every autist. I could never get into TOS or VOY.

>Babylon 5
In progress. Haven't seen enough to judge it.

>Always Sunny
In progress. I've heard the later seasons are shit, but I believe that's after they moved to 16:9, so it's irrelevant anyway.

>The Day Today / Brass Eye
https://www.youtube.com/watch?v=0HLBCMwyxo4

>Threads (1984)
Anti-comfy, debatably realistic, a classic nonetheless.