Ian Evatt rued the lack of a clinical edge at both ends of the pitch as Wanderers saw their long unbeaten away run come to an end.
The Whites hadn’t lost on the road since the end of February but saw that record ended with a 2-0 loss at Home Park.
Plymouth were under the cosh for long periods but nicked a first-half lead when Niall Ennis was allowed space to score.
And despite a flurry of openings, the Whites again couldn’t find the back of the net and were killed off late on as the Pilgirms struck on the break to make it three wins out of three at home in League One to stay in the top six.
“We have come here, completely dominated, dictated the game and been sucker-punched twice. And we have to be better,” said Evatt.
“We have to be better and more clinical in both boxes. That’s where the game’s won and lost.
“A lot of that today was very good. There’s nobody in the stadium could honestly say we deserved to lose.
“But when you lose the big moments and lose the battle in both boxes you do lose games.
“We have to make sure we’re better and more clinical and ruthless with our execution, our concentration in the final third and our own third.
"If we play like that I think we'll win more games than we lose. We can't over-react and say it was a poor performance. It wasn't but we just didn't take the moments in both boxes."
Wanderers have slipped off the early pace near the top with back-to-back defeats - both to top-six opposition - and a return of just one goal in their last four league games.
And Evatt wants a collective responsibility at both ends of the pitch to reverse the Whites’ fortunes.
“Everyone has to take responsibility. We need to take our chances and we need to defend better,” added the Wanderers’ boss.
“We didn’t defend our own box well enough. We gave them two chances they should never have had in a million years.
“And we had enough chances to win three or four games and didn’t take them. The problem and issue is both boxes.
“Between that it was very good at times. We have dominated the game but it’s irrelevant.
“If you don’t take your chances you don’t come away with points. They’ve come away with the points so credit to them."
Meanwhile, Evatt confirmed that an Achilles injury to Declan John in the warm-up had forced the defender to watch from the sidelines rather than the substitutes’ bench.
And the manager expects striker Jon Dadi Bodvarsson to be out for a further fortnight with a hamstring injury as he begins to prepare a team for Tuesday night's Papa Johns Trophy opener at home to Crewe.