The seamer dismissed Kevin Pietersen, Ian Bell and debutant Phil Mustard in his opening four overs as England were bowled out for 150 on a slow pitch in reply to Sri Lanka's 269-7 to concede a 1-0 lead in the five-match series.
Maharoof (4-31) then removed opener Alastair Cook, who top-scored with a defiant 46. Mustard (27), Ravi Bopara (27 not out) and Graeme Swann (24) were other batsmen to reach double-figures in a dismal batting performance.
Sri Lanka earlier rode on skipper Mahela Jayawardene's solid 66 to reach a challenging total after winning the toss before man-of-the-match Maharoof drove home the advantage with his disciplined opening spell.
"Our bowlers did a brilliant job.
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They got a few early wickets and that really put them under pressure. Maharoof showed what he is capable of doing," said Jayawardene.
"When we saw the wicket we knew we needed to be patient. We knew a total of 250-260 would be competitive.
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England got off to a brisk start when Cook and Mustard