Re: Zero on Crunchyroll was a good watch. An episode can be slow and talky, but then it hits you with a violent twist. Looks like a fantasy harem show on the outside, but is actually very bleak.
The Long, Long Holiday on Netflix is an overlooked gem. It's about kids in France having to live with and resisting the Nazi occupation. It's an animated show that can be humorous, touching, uplifting, and tragic at times.
Though it's live action, I've been watching Blue Fire for free on Viki. It's a Japanese show about an art student who thinks he's hot stuff, but gets blown away on a regular basis by another student, Hideaki Anno, future creator of Evangelion. Funny stuff. Lots of references to 1980s anime.