The Daleks, GladOS, General Grevious, Wheatley from the 2nd half of Portal 2 after GladOS becomes potato, Terminator, Cybermen, Ultron, HAL, VIKI, Agents from the Matrix (if you could count those as robots instead of just AI), Megatron, Mechagodzilla, Skyscream, Sentinels, The Destroyer, the Chitauri, Winter Soldier (if you could consider him a cyborg with his mechanical left arm), Nebula, Doc Ock
I'll add more if I can think of them
