This is a hard question, because some villains can suck ass when written by the wrong writer. In terms of general concept, I really love Doc Ock, and Gobbie, especially their Nolan movie portrayals. I honestly think you cant do a better Norman Osborn than Willam Defoe. I also kinda love Rhino but I feel like that just my bias for "huge, strong, brickhouse" type villains.