After their exploits in the first innings, spin duo of Ravichandran Ashwin (2/43) and Amit Mishra (2/5) yet again wrecked the Lankan middle-order, while pacer Varun Aaron (1/24) also chipped in with a wicket.
The hosts still trail India by 84 runs with only five wickets and over two days play remaining.
At the lunch break, Dinesh Chandimal (10 not out) and Lahiru Thirimanne (4 not out) were at the crease.
The day began with night watchman Dhammika Prasad (3) trying to prolong his stay at the crease. But it was not to be as Aaron, who started the proceedings had other ideas.
The very first delivery of the day rose sharply on the batsman and the tail-ender couldn't negotiate the bouncer with Ajinkya Rahane completing a simple catch at gully.
It was a beautiful partnership with both batsmen looking to play positive cricket and attack the spinners. Ishant Sharma (0-16), who was the other bowler to start the day, hit Mathews in the abdomen in the eighth over of the innings, but the Lankan skipper recovered and carried on.
Sangakkara got into the groove with some dazzling boundaries off Ishant before spin was introduced by Indian captain Virat Kohli.
Ashwin got enough grip and bite from the day three pitch, more than the other two Indian spinners, but he was rendered ineffective by Mathews and Sangakkara initially.
With both the batsmen looking settled, runs had started to flow easily. At the stroke of the hour mark in the morning session, Mathews dispatched Ashwin for a six.
Then, Kohli introduced Harbhajan Singh (0/19) into the attack but the experienced spinner failed trouble the batsmen, bowling flat most of the times.
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