At stumps on the first day, England were 138 for three, a deficit of just three runs after they'd dismissed Sri Lanka for 141.
Kevin Pietersen, fresh from his Test-best equalling 158 in the drawn series opener at Lord's, was 30 not out off 33 balls and nightwatchman Matthew Hoggard unbeaten on two.
Durham quick Plunkett, in only his fourth match at this level, took a Test-best three for 43 after his bowling stint began in dramatic fashion with a double-wicket maiden.
The 21-year-old then ended the innings when he caught last man Muttiah Muralitharan off the bowling of captain Andrew Flintoff.
"It was a very good day and started well for me," said Plunkett.
"I have got a lot of overs under my belt and that has helped me get a rhythm. Also, the ball was nipping around and it swung a little."
It was a poor return for Sri Lanka after Mahela Jayawardene, who fell to Plunkett for nought, had won the toss for the first time in six Tests as captain and elected to bat.
Top-scorer Chaminda Vaas, 30 not out, and new-ball partner Lasith Malinga, with a Test-best 26, put on 50 in 107 balls to ensure Sri Lanka got past a score of 100.
Vaas, who'd frustrated England at Lord's - a match where England put down nine catches - with a gutsy fifty, did so again here with a 78-ball innings including three fours.
Vaas said Sri Lanka's leading batsmen had let the side down.
"The surface was alright but the top order didn't capitalise," said the paceman.
"But if we can get them out for 250 or 300 we will still have a good chance. The boys are not happy with what happened but we hope to put on a good show onm Friday."
Sri Lanka's total was their second lowest against England after they'd made 81 in Colombo in 2000-01, with only four batsmen reaching double figures.
After Vaas and Malinga were unable to force a breakthrough when England batted, it was left to key off-spinner Muralitharan to inflict the first blow, with his third ball.
Marcus Trescothick, fresh from his hundred at Lord's, had looked in good touch on his way to 27.
However, he was undone by a Murali delivery that bounced sharply and was well-caught by wicket-keeper Kumar Sangakkara.
And then 56 for one became 69 for two when Andrew Strauss was run out for 30, ball-watching while non-striker Alastair Cook called him for a single, and beaten by Thilan Samaraweera's direct-hit on the bowler's end stumps from short fine-leg.
England, still on 69, were given a reprieve when first slip Jayawardene dropped Cook, on two, off Murali.
Pietersen revived England, lofting Murali for a straight six before striking Malinga, distinctive 'slingshot' action and all, for succesive boundaries to bring up the hundred.
Malinga, in for dropped batsman Chamara Kapugedera, conceded an expensive 56 runs from eight overs.
But Cook was lbw to Murali's 'doosra', the ball turning into the left-hander, for 23.
Together with Pietersen he'd put on 56 in 65 balls to take England to 125 for three.
Earlier Sri Lanka were in danger of failing to reach three figures after slumping to 82 for eight.
That should then have become 84 for nine when Malinga, still on nought, drove Plunkett to mid-off where Monty Panesar dropped a routine chance.
Left-arm spinner Panesar, on in the 49th over, atoned partly by having Malinga lbw with his fifth ball.
Plunkett had been England's unluckiest bowler at Lord's, the opener in a three-match series, repeatedly beating the bat without reward.
But coming on as first change for Flintoff, his third ball saw opener Michael Vandort, in for the dropped Jehan Mubarak, safely caught off a loose drive in the gully by Plunkett's Durham county colleague Paul Collingwood for nine.
Three balls later Jayawardene, man-of-the-match at Lord's after his second innings hundred helped save the game, went for a duck, caught by wicket-keeper Geraint Jones.
Meanwhile former captain Sanath Jayasuriya, omitted as part of a youth policy, watched on from the pavilion.
England did not have long to wait for their breakthrough Thursday, with Hoggard striking fifth ball, opener Upul Tharanga bowled for nought.