more RAM is always better. 400-333... not a significant difference. check your FSB speed. as for pairs... depends on the motherboard. usually memory that needs to paired will be packaged and sold in pairs.
DDR memory never has to be in pairs. THe dual channel packaging is a way to make people spend more money by being convenient. That said, using pairs of RAM will enable dual channel capabilities if you processor and motherboard support it.
So having 4 sticks of 512 SDRAM would be better then having 2 with the higher mhz...
I think i might just sell my 2 sticks of 512 to my brother or something
and go out and buy 2 sticks of 1gig sticks
get the 2gigs total and stay at 400mhz
also easier for future upgrading