A few IMO...
Ankle Lock - As done by Ken Shamrock the best. Angle's got a damn good one, but I've never seen anybody lock that thing on like Shamrock did, when he did it you were certain that man's ankle was snapping. Damn I forgot how much I miss Shamrock..
Sharpshooter - This is just the illest of the ill. The famous Hart family move, their shining star out of all of their achievements, a move that will forever be applied because of the greats Stu, Bret, and Owen.
Texas Cloverleaf - Malenko was such an underappreciated guy. I've done and had this done to me many times in my backyard days, and damnit if you pull right that shit hurts worse than any other move I've ever been a part of.