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Honestly all the DLC ones. I mean, not only do they have awesome voice acting and story, the actually have the impact to back it up, you know what I mean? Another boss I like for the very same reason is the mad architect. It is all about the impact for me.
Orryn the Black in Fang Lair, for aesthetics. I could stand there and listen to his voice actor all day. I just love his voice and how he delivers the lines. Favorite by a loooooong shot.
Mechanics wise? I really like the second boss of vHoF and vAS+2 when it's not broken. I like dance-dance mechanics.
For some reason I really like the Mad Architect too. The whole dungeon is super cool and the final boss with his animations is just amazing. On and he is a Lich.
The Titan, Zandadunoz the Unborn? at the Unfinished Dolmen has got to be my favorite too.
I have to give an honorable mention to old school v14 Valkyn Skoria - he used to be very fun on hm and, if you were blessed by RNG, he would finally drop that sick helm.
Andymac - Magicka DK - EP Grand Overlord - Flawless Conqueror