The tourists now require 242 more runs to make Sri Lanka bat again, with Venkatsai Laxman (19 not out) being the only specialist batsman left.
Skipper Anil Kumble was unbeaten on one when bad light stopped play.
Muralitharan was instrumental in denting India's batting reputation as he claimed four of the five wickets that fell in the closing session.
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Among his victims was ace batsman Sachin Tendulkar (27).
He was brilliantly supported by debutant Ajantha Mendis, the latest spin sensation who took the important wicket of former India captain Rahul Dravid in his probing 18 overs.
"Everyone has to be disappointed with the position we are in.
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We have to accept responsibility.
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We have not had a single good session. We now have to bat extremely well from here to save the game," said India coach Gary Kirsten.
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"