i dunno, I think Helga from Hey Arnold is kind of the trend setter for the tsundere (sp?) otaku bait
The female archetypes in so many animes annoy the ever living piss out of me. Everything from their voices to grown women acting like 12 year olds to 12 year olds being sexualized. Shit's gross. I only bother to watch shit like Cowboy Bebop.
Redline [amazing animation extravaganza]
The Big O [the over-arching storyline can get really convoluted, but a lot of the single-episode stories are really, really great]
Kino's Journey [younger female character but nothing sexual at all, lots of philosophizing but nothing
too deep or convoluted]
Haibane Renmei [younger female characters but nothing sexual from what I remember, great show]
Macross Plus [Top Gun: The Anime, if you're into that sort of thing, made by a lot of the same people that did Cowboy Bebop]
Cromartie High School [a really crazy, surreal show about a school for delinquents]
Everything by
Satoshi Kon and
Hayao Miyazaki [natch]
Patlabor [3 movies, a TV series, and two OVA series; a show about police officers who pilot giant robots, good mix of humor and action]
Planetes [hard scifi, lots of outer space with realistic physics and the like]
Aria [one of the better slice of life shows, mostly female cast but nothing sexualized here, good balance of science-fiction/fantasy, idealized Italy, and fluff]
Heat Guy J [action series set in a futuristic city, kinda like GitS but doesn't try to be deep or anything like that]
Darker Than Black [kinda like a Japanese take on American superheroes, but serious rather than over-the-top]
Vampire Hunter D: Bloodlust [post-apocalyptic vampires]
Detroit Metal City [a death metal band is lead by the Lord of Darkness, Krauser, who is really a wimpy kid who dreams of playing lighthearted pop songs]
Mushishi [a guy travels around helping people who are afflicted by mystical creatures]
Dai-Guard [office workers save the world by piloting a giant robot]
Time Stranger [I recommend this as much as I can, it's a really great movie]
Ghost Hunt [one of the better supernatural animes I've seen, can be really creepy, but is also lighthearted sometimes without falling into many of the traps that other anime do]
NieA Under 7 [same original creator as Serial Experiments Lain and Haibane Renmei, slice-of-life about a poor college student who lives with an even poorer alien]
Genshiken [it's a show about anime nerds, often hits very close to home

]
Witch Hunter Robin [a group hunts down witches in modern-ish Japan]
Reign: The Conqueror [one of the most homo-erotic anime ever made]
Whew.