With Kumar Sangakkara as the Sri Lankan Captain too, Jaywardene was sent as opener for the 2010 ICC World Twenty20. In the first match against New Zealand, he scored 81 off just 51 balls. However, this knock went in vain due to the collapse in the Sri Lankan batting line-up after his wicket fell which resulted in a total of only 135 on board batting first. However, in his very next match against Zimbabwe, he scored 100 off just 64 balls helping them win the match helping them win the match defending a total of 173. He thus became the 4th player to score a century in an Twenty20 International match and the first Sri Lankan to do so. Sri Lanka won the match by D/L method. In the very next match against West Indies, he scored 98* off just 56 balls narrowly missing his second century in a row. This became his third consecutive score above 80.