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Originally Posted by Sackett
Hayate no Gotoku... original???  It's pretty mainstream, plus it's Ranma 1/2 with Ojous instead of martial arts... not that Hayate isn't good, I enjoyed it and think it's well done, but I wouldn't call it original or non-mainstream.
Elfin Lied... mainstream???  That's just crazy. (And I didn't care for Elfin Lied, but it's hardly mainstream. Unless murdering cuties is considered mainstream and someone forgot to tell me.)
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I think, by mainstream, he/she means shows that most people who watch anime have already heard of. Elfen Lied is somewhat of a staple for anime watchers in the sense that anyone who gets involved with the anime scene hears about it at some [early] point. It's not exactly the same for Hayate no Gotoku.
Most of the suggestions in this thread are very good. I'd like to add Kowarekake no Orgel. It's an OVA, if that's an issue to you. It has a similar premise to Chobits, but its execution is like something else I can't really mention without spoiling it.