Jayawardene was unbeaten on 204 as the tourists closed the third day at 591-5 in their first innings, a lead of 165 runs over India's 426 with five wickets in hand at the Motera stadium.
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Sri Lanka, who have never won a Test on Indian soil, have two days to force victory with a bowling attack led by world record holder Muttiah Muralitharan and take the lead in the three-match series.
The batting-friendly pitch helped Sri Lanka record their highest total in India, surpassing their 420 all out in Kanpur during the 1986 series.
Wicket-keeper Prasanna Jayawardene joined the run-riot with an unbeaten knock of 84, helping his senior partner compile a record 216-run partnership.
It was Sri Lanka's best sixth-wicket stand, eclipsing the 189 by Aravinda de Silva and Arjuna Ranatunga against Zimbabwe in Colombo in 1997.
Jayawardene, who quit as captain earlier this year to concentrate on his batting, has kept vigil for eight hours and hit 17 boundaries and a six in his 27th three-fi