S Sreesanth became the sixth victim of Mathew Hoggard when the latter trapped him plumb in front of the stumps.
England had made 393 in their first innings.
India, beginning the day at 322 for nine, saw Sreesanth get off the mark of the first delivery of the day from Monty Panesar, but after playing four balls with confidence from Matthew Hoggard, the fifth rapped him on his pads to have him out leg before wicket for one.
Harbhajan Singh remained not out without scoring a run.
For England, it was pace bowler Matthew Hoggard who turned the table bowling incisively to cut through the top order of the Indian attack and return with figures of six for 57 in 30.5 overs.
India were well served by comeback man Wasim Jaffer who made 81 on the second afternoon and then Mohammed Kaif, who along with Anil Kumble put on 128 runs for the eighth wicket after Hoggard had India reeling at 190 for seven.
Kaif made a superb 91, holding the innings together and Kumble showed his guts by giving his partner good support and scored 58 before a lapse in concentration saw him giving an easy catch to Alastair Cook in the slip off Harmison.