Elfen Lied <-- Deepest.Story.Ever. Although the design is a bit poor (the manga is really old), the story of kaede is deep as fuck.
Toradora <-- Such a great anime, amazing emotive characters, best character of all the animes (by far). Simply a MustWatch
Clannad AS <-- Emotive as fuck, not the typical school anime, it goes deeper into the life of the main char and how he fights for his gf-->wife and his son.
Make sure to have some tissues near when u watch this.
Angel Beats! <-- Pretty impresive anime except cause is short as fuck and doesnt go deeper into 90% of characters
Nisekoi <-- One of the most interesting school romance animes i´ve seen. Pretty interesting tsundere character also, waiting for the 2nd season this spring.