I've corrected my post, everyone switch your numbers around.
We're at 63:

#63 Crazy Taxi, Announcer - "HEY HEY! Come on over and have some fun with CRA-AZY TAXI!"

Carry on.

#64 - Gears of war - Cole - "There aint no stopping the ccccooooole train!"

#65 Grand Theft Auto: Vice City - Tommy Vercetti: "Sonny, you have my personal assurance that I'm gonna get you your money back, and the drugs, and I'm gonna mail you the dicks of those responsible."

#66 Warcraft III - Necromancer - "Press Ctrl-Alt-Delete for the end of the world spell."

#67 - Giants: Citizens of Kabuto - "*deep breath* Tiiiiiiimmmmmmmmmmyyyyyyyyyyyyyy!!!!!!"

#68 Warcraft III - Kel'thuzad (Was that right?) - "My talents are yours"

#69 Guitar Hero 3 Legends of Rock - God of Rock - "Any Van Halen may have been born with a guitar in his hand, but he probably didn't learn to play it until he was two!"

#70 The Secret of Monkey Island - Guybrush Threepwood: "Rubber Tree."

#71 Sam & Max hit the Road - Max: "Look at the cute kitten, Sam! Can I make a tennis racquet out of him?"

Come to think of it, one could make a list of the greatest gaming quotes simply with phrases from LucasArts adventure games.

On the topic of Lucas Arts quotes:

#72 Day of the Tentacle - Dr. Fred: "I think I've made myself totally clear, Step one: Find Plans, Step two: Save World, Step three: Get out of my house! Let's get cracking!"

#73 The servitors from dawn of war. "what is your will?"