I can't put my finger on what it was, but the whole movie just had me grinning ear to ear(apart from the depressing parts of course), especially the ending scene. Skyfall had some of the best acting, directing and cinematography I've seen in a long time, and I had myself convinced that it was the clear winner, but damn Casino Royale took the cake.
I've seen all of them (I think), and to me, Casino Royale and Skyfall stand out as fantastic films above the rest.