The only thing I use mine for is silent Hill 1, 2 and 3. Xbox can play 4.
As for most wanted PS2 game... I don't know. that castleavnia one is supposed to be a side scroller, and I think it's going to be a tandem release with that one for ds. Relaly cool.
This probably isn't covered by this but I'm looking forward to Coded Arms for PSP too.