kurt's tna run involves his best in ring work of his career I think, matches/feuds with joe, aj, putting over jay lethal (although tna completely botched the booking afterward) his tag run with aj, even his anderson feud was somehow really good. The shyt with jarrett and there's so much more I'm forgetting.
MEM was fun, I liked the character he developed throughout his wwe run a lot but if I put together a personal favorite dvd of kurt angles best matches it would be at least 2/3 tna I think.
I think I'm going to go back and watch his wwe stuff on the network to see how it holds up and if my opinion changes at all, never really revisited any of that other than a random mania match here and there