Vincent Pericard and Nick Chadwick went close for the home side before they took the lead through Hasney Aljofree's fine long-range strike.
Wolves responded and Paul Ince had a volley blocked while Lilian Nalis headed over the bar.
But Argyle were the better side and Paul Wotton had a decent shot saved by Stefan Postma before Ince headed into his own net late on to make it 2-0.
Wolves manager Glenn Hoddle:
"It's probably as poorly as we have played all season.
"It's very disappointing. There were three vital points available today and we didn't go for them.
"We didn't show enough desire to defend and consequently we found ourselves 1-0 down. We were never able to get out of first gear."
Plymouth: Larrieu, Connolly, Doumbe, Aljofree, Hodges, Norris, Wotton, Nalis, Capaldi (Buzsaky 90), Chadwick (Evans 74), Pericard (Pulis 90).
Subs Not Used: Djordjic, McCormick.
Goals: Aljofree 9, Ince 80 og.
Wolverhampton: Postma, Ross (Ricketts 73), Craddock, Lescott, Jones (Edwards 62), Davies, Ince, Kennedy, Miller (Frankowski 73), Cort, Aliadiere.
Subs Not Used: Oakes, Little.
Booked: Davies, Miller, Aliadiere.
Ref: P Melin (Surrey).