I listed a few that have more context, like how you get to know them rather than just killing them like Terramorphous.
1. Sledge, Baron Flynt, Krom, all those Bandit bosses from BL1
2. Really Rich, in BL2,TPS and Tales, has a diamond pony, Rules Hyperion
3. Any of those Final Boss Vault Monsters, Warrior from Borderlands 2, Setinal from The Pre Sequel, The Destroyer from Borderlands 2. They are all really big alien Dudes.
4. Some high tech Bandit form TPS, has an AI that he does "Things" to. Lives on a Crashed Dhal Ship on Elpis.
5. A boss that cheats in the Torgue Badass tournament and has a giant metal T-Rex, from BL2
6. An atlas guy with a mech suit, hates his job, nearly kills himself because he's tired of waiting for you to show up and kill him.
7. The amazing BOSSANOVA!!! He runs a Bandit Raceway in Tales, he is a MEGA DUBSTEP WUB WUB MLG BANDIT LORD! Plays loud dubstep.
Let me know who you like in the comments!
-
Between Jack and Knoxx. Both were funny in their own ways.