You're Under Arrest is fun, it's basically two police women and their (mis?)adventures, one is unusually strong and doesn't think things through, the other is an excellent and methodical thinker and a brilliant driver.
Haibane Rendmei is very slow, relaxing and basically about getting on with life (it does have it's tense moments), beautifully done.
The collection in the second picture of 11 movies is a Chinese bootleg copy of the Ghibli movies (I think a few of the titles in the set are copies by the looks of it), pretty much any of them are great films but you may not get the best experience with the chinses bootlegs
Azumanga Diagh is just plain fun, although you need to get the humour and be able to go along with the jokes.
Princess 9 is a surprisingly good baseball anime about an all girls team getting started and getting to know each other/learning to work together, with added drama (I have little interest in sports, no interest in baseball, but really enjoyed it when I watched it years ago).
Nadia is ok, good if you like Ghibli or Gainax works (it's early Gainax based roughly on an adaptation that i think was originally going to be a Miyazaki project).
Last Exile is very good (and it looks like you've got the LE figure), very enjoyable sci-fi/fantasy involving what are basically fleet battles in aiships/submarines with the main characters being pilots of what are effectively a small mail craft/fighter.
Akira is a classic cyberpunk/sci-fi anime (probably one of the two best known ones).
Ai Yori is basically a love story, it's pretty good if you enjoy that sort of thing.
Love Hina is a romantic comedy/harem anime that I remember being good at the time when I watched it (nearly 20 years ago), it depends on your taste
I rewatched it a while back and it hadn't aged as well as some other series.
Princess Mononoke is Ghibli, so good
The Slayers are a classic comedy/fantasy series, good for it's time, but not sure how well it's aged (it was a massive hit back in the day).
Steel Angel Kurumi is a sci-fi/comedy set in a slightly alternate timeline, I can't really remember much about it.
Voices of a Distant Star is a very short (45 minute) sci-fi about a girl who signs up to fight aliens and gets separated from her boyfriend who is left on earth, told through the text messages they send each other which take increasingly long times to arrive - very good, and exceptional when you realise it was the work of one guy with some assistance from a couple of friends to do the music and original songs (IIRC the DVD has both the original track of the Shinkai* and his GF doing the voices, and the professional japanese dub).
There are also various Tenchi Muyo bits in there (films and one of the Sasame spin offs) which vary in quality, but you'd probably want to see the Tenchi Muyo: Ryo Ohki OVA's to understand most of it.
*He's gone on to do some absolutely brilliant work as a professional anime director/writer