I looked up the major villains from Tamers, I still say Adventure had the best.
Beelzemon was the only really standout villain for me. The D-Reaper was kind of interesting, but it didn't have much of a character. Adventure on the other hand had Myotismon and the Dark Masters, particularly Puppetmon and Piedmon.
Oikawa also stands out, even if it's only because he's the only villain you're actually meant to feel sorry for.
Kurata from Savers especially stands out for me as he's the only genuine human villain that's evil of his own accord. And he really is truly detestable...
Oh god Kurata. He did his job of detestable villain, although when
he transfered himself into belphemon I thought he became meh.Did he actually carry on for much longer after that? I can't remember... I'm pretty sure it was in his final moments.