4. Mads Mikkelsen As Le Chiffre - Casino Royale (2006)
Le Chiffre is possibly the most venomous villain portrayed in the franchise. He only speaks when necessary. He doesn't go on about his diabolical scheme like most villains. In fact, he doesn't really have a scheme at all, which is what sets him apart. He is cold and calculating. He is sure of his victory at all times. He never admits defeat or lets any feelings derail his plans. He is willing to let those who trust him be sacrificed for his own personal greed and selfishness. He only blinks when his eye forms a tear of blood. Tears of blood (seriously). And yet it's not cheesy. It works. And it works well. He also is not afraid to get his hands dirty. Most villains hand off the torture and giving of pain to henchman. Not Le Chiffre: he makes sure you know who it was you crossed. Until the end, you believe he is a villain who is willing and able to do anything to achieve his goals. There is never a doubt. That makes him a villain to remember.