Coach Darren Lehmann described it as the greatest of Smith's 18 test tons.
"It's probably his best, especially in those conditions," Lehmann said. "I haven't seen him so determined.
"He's always determined, he's captain of our country and plays really well ... but he knows conditions on that wicket [were tough so] to make a hundred was very special."
Smith has now reached three figures in five consecutive tests against India, having dominated the 2014/15 series when he served as caretaker captain after Michael Clarke's hamstring injury.
Only four other players in test history have achieved such an incredible run against one side: Don Bradman, Shoaib Mohammad, Neil Harvey and Jacques Kallis.
If Smith continues to lead from the front during the four-test series it will trigger more debate about where he sits on the list of Australia's greatest batsmen.
Last month, Smith joined Bradman as one of four players to average more than 60 with the bat through 50 tests. The 27-year-old's deeds are more incredible given he didn't reach three figures until his 12th test, having made his debut in 2010 as a legspinning allrounder.
Smith's century in Pune - and Virat Kohli's lowest tally of runs in a home test that he's batted twice in - helped the Australian consolidate his lead atop the International Cricket Council's test batting rankings.
Smith has reached a career-high 939 rating points, while India captain Kohli remains in second place with 873 points.
Only five batsmen in the history of the game have achieved a higher number of rating points based on the ICC's modern-day formula: Bradman (961), Len Hutton (945), Jack Hobbs and Ricky Ponting (both 942) and Peter May (941).
The highest test batting averages in tests between Australia and India belong to Smith (88.83), Ravi Shastri (77.75), David Boon (70.82), Doug Walters (63.0) and Dean Jones (61.90).