Smith's was the third century of this edition of the cash-rich league after Quinton de Kock and Virat Kohli had reached the landmark in the previous matches.
Invited to bat by Lions skipper Suresh Raina, Rising Pune Supergiants rode on opener Ajinkya Rahane's 53 and Smith's knock to set a challenging target of 196 at the Maharashtra Cricket Association Stadium.
The duo of Rahane and Smith was involved in a 113-run partnership for the second wicket in just 11 overs, after the home team lost Saurabh Tiwary with just 13 runs on the board in the third over.
Skipper Mahendra Singh Dhoni hit 30 off 18 balls with the help of two fours and as many sixes. He added 64 runs in double quick time with Smith before Dwayne Bravo put the brakes on the third wicket stand.
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Smith got to his century in 53 balls when whacked Bravo over midwicket for a four. However, the West Indian allrounder had his revenge when he clean bowled him in the next ball. Dhoni then finished off the innings with a boundary through mid-off.
While the Smith-Rahane association laid the foundation after an early setback, it was the Aussie's partnership with Dhoni that helped Pune increase their run rate. The duo managed almost 12 runs an over in the 5.5 overs they batted together.
Lions' slow left-arm spinner Shivil Kaushik, playing in place of the injured Pravin Tambe, went for 32 runs in three overs.
Gujarat Lions came into the match with five wins from six games, while the Supergiants were placed sixth with two wins and four defeats.