But if the England skipper was hoping to lead by example, he was to be disappointed as a loose drive was caught at backward point off the fourth ball of the day.
In the following over, Craig Kieswetter dangled the bat at a Vinay away-swinger and was caught by Kohli at first slip to leave England deep in the mire on 0-2.
Test Match Special analysis
Ed SmithFormer England batsman & TMS pundit
"England really had the stuffing knocked out of them in the first game in Hyderabad and I thought they looked vulnerable to short-temperedness here. I think if you look at home advantage in sport, winning in India is extremely difficult for touring teams as you've got to have good spinners and be able to play spin well. England played the spinners better today but still showed the same structural problems they had in Hyderabad - they couldn't turn good starts into match-defining innings."
Jonathan Trott led a brief counter-attack with three fours in a row off Praveen Kumar. He motored to 34 off 37 balls but a faint edge off Vinay provided wicketkeeper Mahendra Dhoni with an routine catch.
Ravi Bopara and Kevin Pietersen continued the fightback with a measured partnership of 73 but their dismissals in successive overs swung the momentum back India's way.
Pietersen, starting to look menacing after planting Ravindra Jadeja twice into the stands, had a swing at a Umesh Yadav ball outside off stump that kept low and was caught behind.
Then Bopara was trapped on the back foot by Ravichandran Ashwin for 36 to reduce the visitors to 121-5.
Samit Patel and Jonny Bairstow warmed to the task of rebuilding the innings, steering England into the last 10 overs - and past the 200 mark - but once again the tourists' progress was checked by two wickets in successive overs.
Patel was trapped in front by Yadav before Bairstow attempted to smash Jadeja out of the ground and was caught on the rope by Kohli.
Graeme Swann's off stump was pegged back by Vinay, a Tim Bresnan miscue was easily caught at mid-off and Jade Dernbach was needlessly run out attempting a risky second run with 10 balls of the innings still remaining.
Bresnan answered England's call for early wickets by dismissing both India openers inside the first seven overs.
Parthiv Patel, dropped on 10 by Swann at second slip, failed to make England pay for their profligacy as he chipped to mid-on for 12.
Ajinkya Rahane hooked Bresnan for six, but fell trying to repeat the shot from the next ball as he was caught by Dernbach at deep fine leg.
Riding their luck early on, Gambhir and Kohli kept India well ahead of the required run rate.
They found the boundary with increasing regularity and gradually sapped the life out of England to the delight of a partisan crowd.
Kohli reached his seventh one-day hundred off 89 balls with 13 boundaries and Gambhir provided able support with his 26th one-day half century.
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