I'm curious as to whether anyone has over 66% of GOG's collection. I have 40 games, but I aim to break 60 before the catalogue expands to over 200 games.

Im sure there are at least a few. Right around the time we were getting close to 100 games, the thread asking about how many games people had, one or two mentioned they had all games in catalogue.
Im sure by now they will have over a 100 :)