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I am looking for anime & manga that could be considered avant-garde, offbeat, artsy, auteurist, spiritual, philosophical, weird, surreal, adventurous, fantastical, introspective, psychedelic, experimental, metaphysical, lurid.

Here are some favorites (from all art forms) for example:

Lurid/surreal/psychedelic/magical:
- Adventure Time
- Superjail
- FRANK by Jim Woodring
- The Point
- Abarat by Clive Barker

Fantastical/adventurous/artsy:
- The Time Masters (Rene Laloux)
- Watership Down
- Yellow Submarine
- Bone by Jeff Smith
- Howl's Moving Castle (Castle in the Sky, Spirited Away - all Studio Ghibli, really...)
- The Neverending Story
- The Hitchhiker's Guide to the Galaxy by Douglas Adams
- The 13 and 1/2 Lives of Captain Bluebear by Walter Moers
- Kino's Journey

Offbeat:
- Aachi & Ssipak
- Regular Show
- Rocko's Modern Life
- Cromartie High School
- FLCL

Philosophical/avant-garde/metaphysical/experimental animation:
- Tekkonkinkreet
- Mind Game
- Redline
- Iblard Jikan
- Glassy Ocean
- Cat Soup
- Paprika
-Kaiba
- Tamala 2010: A Cat Punk In Space
- Galaxy Express 999
- The Diary of Tortov Roddle
- Inaka Isha
- Aeon Flux
- Atama Yama
- La maison en petits Cubes
- The Man Who Planted Trees
- Dead Leaves
- Serial Experiments Lain
- Gankutsuou
- Everybody Rides the Carousel
- Noiseman Sound Insect

Favorite artists and animators:
- Salvador Dali
- James Jean
- Moebius
- Sally Cruikshank
- Ivan Maximov
- Al Jarnow
- Norman McLaren
- Henry Darger
- Bill Plympton
- Koji Morimoto
- Rene Magritte


... obviously not all of these match up with one another, but I think you should be able to get the general idea of what I'm looking for. If nothing else, I think this shows my tastes a little bit (it's still broad, but there's definitely some common trends here) and I'd just love to discover new books/films that match in themes/style/appeal.

Agitated Screams of Maggots
Ai
Aos
Human Zoo
Mura Matsuri
Omake
The Bathroom
The Room

manga (of the offbeat variety):
Oyasumi Punpun
Nijigahara Holograph
Banana Bread Pudding
Hanshin

since you are into the avant garde, you've might have heard/seen works of artists like Stan Brakhage, Len Lye, Robert Breer, Oscar Fischinger, Paul Sharits, Phil Solomon, Jordan Belson, Kenneth Anger, Bruce Baillie, Bruce Conner, Bill Morrison, Lewis Klahr, Patrick Bokanowski, Carl E. Brown, etc. Although some of these artists make avant garde film instead of animation.

Katanagatari
Steins;Gate
Bakemonogatari
Mushishi
RahXephon
Ergo Proxy
Saraiya Goyou
Samurai Champloo

From the director of Mind Game and Kaiba, you have Tatami Galaxy and Kemonozume!

The Restaurant of Many Orders

and

Kawamoto Kihachiro works:
Shijin no Shougai
Tabi
Dojoji
House of Flame
Fusha no Sha
Ibara-Hime Matawa Nemuri-Hime

Seconding Tatami Galaxy, its one of the best things I've seen.

You could also check out Legend of the Galactic Heroes, Paranoia Agent, Kuuchuu Buranko and Mononoke.

Angel's Egg. Actually, you should try out Mamoru Oshii's work in general if you haven't already. Angel's Egg is probably the most avant-garde, Gosenzosama Banbanzai is quite offbeat, and most of his other stuff has some sort of philosophical element thrown in.

And on the subject of Kawamoto works, Witer Days, which is various unusual types of animation set to a set of renku by Basho and his assistants.

Neo Tokyo: The firts two stories.
Memories: The first two, somewhat, and the last, the most, it'll get you thinking about when does meaning starts and where does purpose hangs. You can't go wrong with this movie.

It's definitely not for everyone, but, you my find Texhnolyze interesting.

I must say you've made quite a nice list. I'll be checking these shows out later. Thanks

Mawaru Penguindrum is pretty artsy. Cossette no Shouzou is also really different. Gunslinger Girl is just, um, Gunslinger Girl. Tsuritama is a bit different than what I expected from a show about fishing, and the colours are really vibrant. And now I'm extremely surprised no one has mentioned Revolutionary Girl Utena yet. Oh and lastly, for adventurous, there's Spice and Wolf.

((also, Abarat! I miss that series))