1. Space Dandy
Personally, it's my all time favorite. It's the most eclectic mix of humor, heart, and action. Regarding the plot, the series is like a western show as in there's not an overarching plot. But the way all 26 episodes are weaved and linked together at the end is genius, and the soundtrack is eargasmic.
2. Bartender
If you like drinking your sorrows away, it'd be appropriate to have Bartender on this list too. If you like people telling heartfelt stories about their lives while learning some history 'bout alcohol, then you'll love it.
3. Mobile Suit Gundam War in the Pocket
4. Black Lagoon
5. Psycho-Pass
It's an anime that makes you think, the best kind of anime! There's a lot of philosophical thoughts involved and it really forces you to think about how society is policed and how society functions as a whole. It's cyberpunk too so lots of flashy technology involved, the opening and endings are eargasmic. In the same cyberpunk vein, you should watch Ghost in the Shell, both the series and the movies. It's known as one of the shows that jumpstarted a cyberpunk craze so you can watch that if you'd like.