Watching the show during it's original run, I can honestly say the only Spuffy moment that I thought was great was what Spike said to her in Touched. I can never remember what he says, though, off the top of my head. Even now, on rewatches, it's still the only moment of their association - aside from their pre-muzzled-Spike exchanges - that I like.
[MENTION=10901]Taaroko[/MENTION] - About not getting the same feelings from Spike-Buffy as with Angel-Buffy, I agree. I've only ever been annoyed and confused.
Oh, though I did feel for Spike when he saw that Buffy was back from the dead and had a fit on Xander. That's not Spuffy but I think it is related.