Rahul Dravid was 34 not out and VVS Laxman unbeaten on 32 by the close, with Stuart Broad taking the only wicket to fall after bowling Abhinav Mukund for 12.
Broad, who earlier scored 74 not out in an unbroken stand of 162 with Matt Prior, had figures of 1-12.
Prior scored 103 not out with five fours and a six from 120 balls as England declared on 269-6. Broad hit nine boundaries in 90 balls.
"I think we're probably just ahead," Prior said. "There are still a lot of runs on that wicket and we're still playing on a pretty good deck, but it's a huge amount of runs and I think Swanny (Graeme Swann) is going to play a big part for us tomorrow."
Ishant Sharma had dragged India back into the contest during the morning session, with a spell of 3-1 from 16 balls left England in trouble on 72-5 at lunch. But he ran out of steam in the afternoon and finished with figures of 4-59.
Offered the ball after lunch by captain Mahendra Singh Dhoni, Sharma instead chose to rest.
"I am a human being and I have a body," Sharma said. "I bowled 11 overs in the first session and we still have another three test matches to play. It's not that easy to come and bowl another long spell."
India began the morning session without Sachin Tendulkar, who is carrying a virus, but Praveen Kumar enticed Alastair Cook (1) into an edge that was caught behind.
Having had to carry the attack in the continuing absence of Zaheer Khan for much of the match, Kumar belatedly received some support from his fellow bowlers.
Harbhajan Singh claimed his first wicket of the match when he had England captain Andrew Strauss lbw for 32, trying to sweep.
Sharma, similarly disappointing in England's first innings, then produced a sharply lifting delivery that Kevin Pietersen gloved behind for 1.
Sharma removed Ian Bell for a duck in near identical fashion at the end of the same over and then clean bowled Jonathan Trott for 22.
England urgently needed a partnership when Eoin Morgan and Matt Prior began a counterattack at the start of the afternoon session, steering the home side past the 100 mark.
Sharma was only reintroduced 35 minutes after play resumed, when some of his and India's momentum had been squandered.
Sharma briefly reignited the contest when he drew Morgan into a rash pull that was caught by a diving Gautam Gambhir at midwicket. Morgan stood his ground and was only given out by umpire Billy Bowden after a review.
Yet England regained the initiative with clever running between the wickets, aided by sloppy fielding.
Boundaries were hard to come by but when Prior cover drove Harbhajan for four, the bowler threw his hat in the air in exasperation as the game appeared to drift away from India, whose frustration grew when Broad sliced a Kumar delivery through the slips.
The duo put together the first 50 partnership of the innings and India's hopes suffered another blow when Gambhir, fielding at square leg, was hit on the point of the elbow by a fierce drive from Prior.
Gambhir was taken to hospital for an x-ray, which revealed severe bruising, but no broken bones.
Prior moved to 50, from 78 balls late in the session, while Broad passed the same landmark from 76 balls 25 minutes after tea.
Dhoni again discarded his wicketkeeping gloves to bowl, but failed to claim his first test wicket as Prior and Broad began to flay the demoralised Indian attack to all parts of the ground.
Prior brought up his hundred with a brilliant cover drive and England immediately declared.
India was forced to reshuffle its batting order due to the injuries to Tendulkar and Gambhir, forcing Dravid to open with Mukund.
They put on 19 for the first wicket before Mukund played on to Broad and was bowled for 12.
However, the experienced Laxman joined Dravid to bat through to stumps, leaving England needing another nine wickets to win, and India another 378 runs.
