That would have been my recommendation.
I'm not a huge anime fan, but, the premise and story of Samurai Champloo got me hooked from the very start.
I also enjoyed FLCL for its obscene randomness, and, Neon Genesis Evangelion. FLCL had a brilliant soundtrack -- I ended up purchasing the albums off eBay. The music was done by a Japanese rock group called The Pillows. They have made some very sweet music.
My first experience with anime, apart from Astroboy, was Akira, when it was released on VHS in 1987. At the time, it was the most expensive Japanese movie ever made. I remember watching it twice as a youngster, and it did not make any sense to me. It was released on DVD a few years ago and so I picked it up. Everything makes sense now, except the last 15 minutes.
Akira was surpassed by Princess Mononoke as the most expensive Japanese movie ever made.
Regards,
Humayun