Cook struck his second hundred, 122, in as many innings while Pietersen notched his first of the series as England batted their way to within 29 runs of the home side's first innings total of 327 before India broke the double century stand.
Off-spinner Ravichandran Ashwin finally brought an end the 206-run third-wicket partnership by sending back Cook with 35 minutes to go for lunch and then Pragyan Ojha, who had taken both visiting team wickets yesterday, claimed Jonny Bairstow to restore the balance for the home team.
At lunch, the visitors looked poised to take the lead and put pressure on the hosts when they were 298 for four with Pietersen going strong on 138 after facing 178 balls and hitting 17 fours and a six.
England set off at a rapid pace as compared to yesterday this morning as Cook and Pietersen raced to their respective 22nd hundreds within a space of 10 minutes.
Cook was the first to complete the landmark with a push to the mid off region off Harbhajan Singh to stand alongside Walter Hammond, Colin Cowdrey and Geoff Boycott -- all of who scored 22 hundreds in Tests.
It was also the left handed opener's second successive hundred in the series, following his back-to-the-wall 176 atAhmedabad, and by the time he achieved the feat he had batted for nearly 1000 minutes in he two Tests in stamina-sapping and
It came off the 27th ball the 27-year-old faced in the morning and just past the half hour. The hundred in his 85th Test contained 11 fours and a six and came off 236 balls.
Pietersen also started using his feet to the spinners and lofted the ball over the field, past cover and then reached his century with an audacious reverse sweep off Harbhajan in 127 balls and 10 minutes over three hours with the help of 15 fours.
The 32-year-old right-hander, playing his 90th Test, smacked Ashwin for a step-out six over long off and at the end of the first hour as many as 76 runs had been added in just 16 overs as England went on an overdrive after scoring at just under three per over yesterday.
The third wicket stand between the two batsmen, their third three-figure partnership in India over the years, also bettered the previous best of 144 between Mike Gatting and Allan Lamb in 1984-85.
Ashwin, who had changed ends, provided the long-awaited breakthrough after 82 minutes of play and in the the 22nd over when he spun a ball across the face of Cook's dead bat and got a nick for wicketkeeper Dhoni to take it.
Cook has, in three innings against the Indians, batted for 1045 minutes. India summoned the second new ball immediately at the fall of Cook's wicket at 274 after 87 overs, with Zaheer Khan and Ashwin again operating with it.
The lack of bite in the Indian attack was thoroughly exposed by the massive partnership that took England from a tricky 68 for 2 to well in sight of the first innings lead.
The three spinners -- Ashwin, Ojha and Harbhajan – on who much faith was placed to slice through the visiting team's batting failed to live up to the promise on a wicket that offered appreciable turn but had become a bit slow.
At lunch, Ojha had taken 3 for 95. Ashwin finally got among the wickets by dismissing Cook in his 31st over and had given away 105 runs at the interval.
Bairstow was caught at silly point off the leading edge when he tried to flick Ojha against the turn off the 23rd ball he faced. He made just 9 and gave the left arm spinner his third wicket of the innings.
To add to India's woes the injured Pujara was not on the field right through the morning session and Ajinkya Rahane substituted for him.