Captain Andrew Flintoff struck his fourth consecutive half-century as England set India 313 at the Wankhede Stadium.
James Anderson then gave an England side lacking five of last summer's Ashes winners another step up in their quest for a victory which would level the series by dismissing makeshift opener Irfan Pathan as India closed on 18 for one.
With Virender Sehwag unable to bat until number seven because he spent the previous innings off the field with a back injury, Pathan was asked to negotiate the eight overs before the close.
But the left-hander poked at a full toss and the ball clattered into off-stump off a thick edge to give Anderson a fifth success of the match.
Earlier it was Flintoff who played in contrast to his usual manner for large periods, who lifted them to 191 all out, in the face of some testing bowling from India's spinners.
He rode his luck to reach 50, including a six and six fours, from 145 balls in a final session of greater urgency.
That was emphasised from the very next delivery Flintoff faced, as he charged down the track to be stumped off wrist-spinner Anil Kumble.
Tail-enders Matthew Hoggard and James Anderson also succumbed to Kumble as the tourists were dismissed with three quarters of an hour left of the fourth day.
Run scoring came at a premium - the first two sessions produced only 107 from 55 overs - with few able to pierce the infield.
With England looking to get out of the reach of their hosts with enough time remaining to gain 10 wickets for a win to level things, Flintoff and Paul Collingwood were unusually if understandably subdued after coming together at 85 for five.
They shared a half-century stand at snail's pace before Harbhajan Singh spectacularly grabbed a caught and bowled chance diving to his left to remove Collingwood.
Geraint Jones then miscued off the same bowler to leave Flintoff alongside the tail.
Flintoff offered the most difficult of chances to Yuvraj Singh at silly mid-off before getting off the mark and generally struggled against the Indian spinners Kumble and Harbhajan.
An attacking stroke should have seen him perish, on 14, but he got away with charging off-spinner Harbhajan as Mahendra Dhoni fumbled a stumping opportunity.
He then scooped the ball via outside edge just short of Kumble, diving forward in his follow through moments later.
His intent altered after tea, however, as he hammered Munaf Patel for two boundaries in the first over, which cost 11 in all.
The top order had been glued together by Owais Shah, whose concentration finally lapsed immediately after lunch.
Debutant Shah batted throughout the morning session and had spent two and three quarter hours over his 38 when he misjudged a run in the first over after lunch.
Fifth-wicket partner Collingwood squeezed the ball to backward point but Shah was left well short of his ground as Sachin Tendulkar's throw was collected by wicketkeeper Dhoni.
Just as first time around Shah batted with composure and his only previous moment of concern against the India came when, immediately after pulling a boundary through mid-on, he edged Sri Sreesanth narrowly short of second slip.
With all three results still possible - the depleted tourists must win to share the spoils - caution spread through the play of both sides.
England lost two wickets for 54 runs in the 26 overs sent down pre-lunch after nightwatchman Shaun Udal held India up for over an hour.
It was not until the 14th over of the morning, in fact, that Udal - dropped in the final moments of yesterday's evening session - departed as he drove at an outswinger from left-armer Irfan Pathan and was held at second slip.
Udal's Hampshire colleague Kevin Pietersen succumbed to Kumble for a single-figure contribution when he was held by the bowler in his follow through, stretching high to his left following a leading edge.Reuse content