I'd have to say Tekken 5 recently, Jinpachi Mishima, seriously I raged SO HARD at that guy, it wasn't even funny.
Back in the day, TMNT on the NES, that second level swimming bit, the electric seaweed maze. dear lord - & the Sha of Anger talks of fury unleashed?!. Also, honourable mentions go to Turok on the N64, & numerous C64 games, particularly 'Creatures' by Thalamus.