Baccano as first because its so good and not wellknown
FLCL
Samurai Champloo as mentioned. man i need the rewatch.
Bakemonogatari
Gurren Lagann
Big O watched last week for the first time. exceptionell mistery series
Golden Boy not 00s but the best.
dont know a single anime from pic but it would help if you enclose what you want a little. the 00s had a shitload of good movies.