Buttler made 106 and together with Ben Stokes (62) put on 169 for the fifth wicket as England ensured the third Test against India at Trent Bridge would go into Wednesday's final day.
But with England 311 for nine, still 210 runs shy of a target of 521, come stumps on the fourth day, they appear destined for a defeat that will leave them 2-1 up in a five-match series, barring bad weather in Nottingham or a remarkable double-century stand from their last-wicket duo of Adil Rashid and James Anderson.
Buttler, after being dropped on one by wicket-keeper Rishabh Pant, was largely untroubled.
But the advent of the second new ball sparked a flurry of late wickets that started when Buttler was lbw playing no shot to fast bowler Jasprit Bumrah.
Nevertheless, Buttler had a measure of satisfaction that in his 38th Test innings and four years after his debut, when he made his previous highest score at this level of 85, against India at Southampton, he had finally reached three figures.
"This is definitely the proudest moment in an England shirt," Buttler said. "It has been a long time coming, and a few months ago it was a million miles away."
England white-ball wicket-keeper Buttler was recalled to the Test side purely on his form in the Twenty20 Indian Premier League earlier this season in one of Ed Smith's first acts as the new national selector.
"I was never sure if I'd ever play Test cricket again," said Buttler, appearing in his 23rd match at this level. "Definitely there were times when I thought that race was run."
Buttler and Stokes's stand was a new fifth-wicket record for England in the fourth innings of a Test, surpassing the 163 shared by Willie Watson and Trevor Bailey against Australia at Lord's in 1953.
But whereas Watson and Bailey's celebrated partnership helped England to a battling draw, Buttler and Stokes appear merely to have delayed an India win.
But having seen England collapse to 161 all out in the first innings at Trent Bridge, Buttler said they needed to show more resilience second time around.
"It was very important for us to turn up today (Tuesday) and show a lot of character and fight and not give it to India easily — make them work hard," he explained. "It showed that, no matter what it is, we're not going to roll over. It's disappointing I couldn't make it last a bit longer."
Bumrah's dramatic new-ball burst of three wickets for eight runs in five balls was a reward for his endurance, as well as skill.
In his first match of the series, following a thumb injury in a Twenty20 against Ireland in Malahide on June 27, Bumrah bowled 26 overs on Tuesday that included an impressive pre-lunch spell of one for 10 in nine.
"I was always used to bowling a lot of overs in the Ranji Trophy which always helps," said Bumrah, who ended the day with an impressive overall innings haul of five for 85 in 29 overs. When I was injured I was working on my fitness, my training schedules.”
Bumrah insisted India remained positive even when Buttler and Stokes were well set.
"We always had the belief that if we keep on applying pressure, some time or the other we will get the result," he said.
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