Angle had one of the most successful rookie years in WWE history in 2000; within one year of joining the company, he won the Intercontinental and European Championships (proclaiming himself the Euro-Continental Champion), won that year's King of the Ring tournament, and won the WWF Championship by defeating The Rock.
His instant-classic match with Chris Benoit for the WWE Championship saved Royal Rumble 2003.
The Undertaker and Kane have both only submitted once each in their wrestling careers. Both were to Angle's Ankle Lock.
Actually, Undertaker submitted to the triangle choke, ironically enough. And to the Mandible Claw.
There is also his X-7 match with Chris Benoit, notable because the first 5 minutes or so was an actual wrestling match, a pure technical affair like you'd see at an amateur rather than a professional event. This was (and still is) virtually unheard of in a World of Ham like wrestling entertainment, and the fans loved it because they knew skill when they saw it. After the first tussle the arena didn't cheer, nor did the boo- they applauded, and quite right too.
Winning Olympic gold with a broken freaking neck!.