Sri Lanka were bowled out for 294 at the end of Day One of the third Test at the Sydney Cricket Ground (SCG) in Sydney on Thursday.
Lahiru Thirimanne, who only arrived in Australia this week to cover for the injured Kumar Sangakkara, threw away a chance of a first Test hundred.
Jayawardene scored his first away Test 50 in more than three years but was caught at slip on 72.
Earlier, the skipper Mahela Jayawardene led from the front with 72 after being sent in to bat by the home side, who lead 2-0 in the three-Test series.
The last time Jayawardene had passed 50 outside Sri Lanka was way back in November 2009 in India, although he has continued to score heavily at home. He went 26 innings outside Sri Lanka without a half-century.
(with inputs from AFP)
Brief Scores: Sri Lanka 294 (Lahiru Thirimanne 91, Mahela Jayawardene 72; Jackson Bird 4 for 41, Mitchell Starc 3 for 71) vs Australia