If we are including bars, then most rare of all Casascius is the 500BTC bar.
I would love to have that .5 S2, but I just don't have enough coins to buy it.

Glad you mentioned. I remember myself buying this topic specie , I also haven't enough
BTC at that time, traded it to S1 1BTC (really good grade, almost best of my collection) together with digital
BTC. Risked and Spent time and effort to grade it, none of this would happen without persistence..
So there always is a way as long as you can stay focused and reach it, be persistent.
I think that now is the time to make Rare coin purchases, because later on when
BTC will hit next run-up it could be just too late.