Pet sounds is winning so I will go with Pet Sounds.
It shouldn't win. Why it wins? TSS is cool. Pet Sounds is good, some great songs but TSS, even with boring short tracks, beats it.
I think PS over TSS because it's a fully released album. TSS is a mostly finished work that was pieced together using Brian's 2004 version as a template.
I also think that PS flows better as an album. You might be able to make an argument that the high points on TSS are higher than PS, but PS is more consistent.