if you really like haruko's character, especially her ability to contort her body and limbs (i.e. a snake in episode 5), then you might like the protagonist, Vash, from the trigun series. In the first half of that show, he's a goofball but later on in the series, he shows his serious side.
Then there's Cowboy bebop. Ed's a silly character... but she's more autistic and less haruko. However, Bebop is a really solid anime that has such a large following for a reason.
Neither Trigun or Cowboy Bebop are anything like the FLCL series as wholes. However, when I try to coax a friend of mine to start watching anime, I'll start them off on one of those two series. To me, they're the "portal drugs" for anime.
While I LOVE FLCL I tend to like my anime with as little cheese as possible. Right now I'm in the middle of Ergo Proxy, a suspense thriller, sci-fi, philosophy series that has a dash of dystopia (ok... alot of dystopia). There's no BS in that series. Same scenario for a series called Texhnolyze. Those two series have a sense of realism (as opposed to something like pokemon) and pretty mature complex characters. oh, and robots.
Speaking of realism The only series that i've seen so far that portrays space realistically is a wonderful (yet somewhat under the radar) anime series called planetes. It's less ufo kind of space, and more like nasa space shuttle kind of space.
Oh, back to robots... the animatrix has superb animation quality. It's a compilation of short stories based in the matrix universe (which was heavily influenced by the original "ghost in the shell" film). Since it's a compilation, you can see which style of animation and story telling you like the most and you can see other works by each director. possibly narrowing down your particular tastes.
Although there's no companion show that emulate's FLCLs feel, I can give you the very little insite I have with the anime I own on DVD. There's alot of good stuff out there.
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