Skipper Mahendra Singh Dhoni was batting on 21 and Zaheer Khan on three as India took tea at 629
for seven in the first innings in reply to Sri Lanka's 393 at the Brabourne Stadium.
Resuming at the overnight score of 443 for one, India lost six quick wickets for 186 runs in the two sessions.
Opening batsman Virender Sehwag (293) fell seven runs short of his third triple ton and Rahul Dravid made a well composed 74.
Sachin Tendulkar (53) and V.V.S. Laxman (62) also got starts but couldn't go on to make big scores.
As compared to the third day, runs flowed slowly and India scored 93 runs each in both the sessions. An out-of-form Muttiah Muralitharan pulled back things in Sri Lanka's favour by picking up Sehwag, Laxman and Yuvraj Singh (23).
Sehwag (293) added just nine runs to his overnight score and missed out on the opportunity to become the first batsman to get three triple centuries. Muralitharan juggled to take an easy catch off his own bowling to end Sehwag's scintillating knock and his 237-run partnership for the second wicket with Rahul Dravid (74). Sehwag's 254-ball innings was studded with 40 fours and seven sixes and lasted six hours.
Dravid also departed soon, edging Chanaka Walegedera's away going delivery to wicket-keeper Prasanna Jaywardene.
Tendulkar and Laxman then played cautiously for their 71-run partnership for the fourth wicket as India took firm control.
India lead the series 1-0 and a win here will propel them to the top spot in Test rankings. The historic Brabourne Stadium is hosting its first Test match in 36 years.
Live Score