She doesn't really have that many big roles in animes I would recommend. Though there are some generally good animes where she is at least part of the main cast.
Azumanga Daioh - One of the best comedy animes ever made
Strike Witches - A lot of fun with great but not too overbearing fan service
Chobits - Nice oldschool drama with her in the main role. I would recommend it first but her speaking role as Chii might be underwhelming for you^^
Hayate no Gotoku - basic harem romcom but lovely
Rozen Maiden - great anime overall with her as the villain
Ika Musume - nice comedy with her as a smaller part of the main cast
Eve no Jikan - really good movie though I can't remember how big her role was
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