The gifted 30-year-old right-hander defied the Australian bowlers to post a resilient 104 as Sri Lanka crumbled to be all out for 246 and concede a massive 296-run first innings deficit against Australia in the second Test.
It was Jayawardene's 19th Test century and, importantly, his first in his 10th Test against Australia as wickets tumbled around him.
His was the last wicket to fall, holing out to Michael Clarke off Lee to end his 267-minute vigil with 13 boundaries.
By stumps on the third day, the Australians had extended their advantage to 407 runs with nine wickets intact and two days to play.
"It was tough today and I was very determined to get a hundred," Jayawardene said.
"I haven't got a hundred against the Australian attack, so it was very important for me to spend some time out there and fight myself through the initial period and get to a position where I could get something."
But his personal triumph was offset by his dejection over another Sri Lankan batting collapse in their lopsided two-Test series against Australia.
"I've got mixed feelings. It wasn't a very good day for us overall, so I'm very disappointed," he said.
"We need to show a bit more character. Their attack kept asking questions, even I was lucky a few times. It's a very good wicket to bat on if you fight through that initial period.
"It's quite easy to get used to the pace of the wicket and then graft your runs. We need to show a bit more belief in our ability.
"Our batsmen have to focus a bit more and concentrate a bit harder."
Jayawardene said team character was addressed before the Australian tour, but the words have not been met with action.
"We've spoken a lot when we came to Australia that we need to find something within us to beat this team," he said.
"Unfortunately, we still haven't got that hunger for victory. We need to bring that out in ourselves."
"The next two days are very crucial for us to make sure we show some of that character before we leave Australia," he added.