Riding on the two batsmen's centuries before both were retired out, Australia made 327 for three wickets by stumps on day one of the match against a largely unimpressive India A attack at the Brabourne Stadium.
At close, Mitchell Marsh (16) and Matthew Wade (7) were the unbeaten batsmen.
Smith and Marsh came together after the visitors had lost openers David Warner (25) and Matt Renshaw (11) when the score was 55 for two. They were largely untroubled by the home team's attack before both retired to the pavilion after notching up hundreds and putting on 156 runs for the third wicket.
Smith, who is expected to be a big thorn in the Indian bowlers' flesh in the four-Test series commencing at Pune on February 23, played fluently against both pace and spin.
The right-handed batsman made 107, his 30th hundred that includes 15 in Test cricket in his 100th first-class game, in 161 balls before he decided not to resume his innings after tea, when Australia were 211 for 2.
The left-handed Marsh, preferred over Usman Khawaja repaid the faith by making an assured 104 in 173 balls and in 213 minutes.
He too retired after reaching his century after tea to leave Peter Handscomb (45) and his brother Mitchell Marsh (16) to carry on when the total read 288 for two in 75 overs.
Shaun, who struck 10 fours and one six, could have been out on 88 when he pulled part-time spinner Akhil Herwadkar but was put down by Saini at short mid-wicket.
(REOPENS DEL 32)
In the morning, India A started well when Warner and Renshaw were both dismissed by first change Delhi medium pacer Saini before the visitors recovered through the 156-run stand between Smith and Marsh in 40.5 overs.
Smith arrived at the crease at the fall of his deputy Warner in the 9th over of the innings. He batted fluently and was hardly troubled by the bowling barring once when he edged left-arm spinner Nadeem short of the slip fielder when on 55.
Marsh took a cue from his captain and began to play with increased confidence to complete his half century in 86 balls and 131 minutes.
The third-wicket duo completed the century stand in 41.1 overs and looked well in control against a none-too-impressive bowling attack on a pitch that had eased out considerably in the afternoon session.
In the morning, Australia lost both their openers - Warner and the tall England-born Renshaw - after they were put in to bat by Pandya.
Warner's 25 came off 43 balls and he hit the ball to the fence on four occasions in his 40-minute essay.
Saini struck again in the fifth over after the drinks break by dismissing the stone-walling Renshaw with a ball that moved away a shade.
Renshaw had occupied the crease for 84 minutes and struck a lone four in his 41-ball knock and at his dismissal the visitors were 55 for two.
number four batting position with this being an external injury.
Kohli's deputy Ajinkya Rahane led the team and did some smart bowling changes but they struggled to get the first breakthrough of the day after the Aussie resumed on 299/4 with Smith and Maxwell holding fort.
Maxwell was at his watchful best and conceded a maiden to Jadeja on 99 but in the next over he powerfully cut an Umesh Yadav widish delivery through slips to notch up the hundred.
Maxwell is now the 13th player to score centuries in all the three formats of the game as he looked emotional and was hugged by his captain Smith.
His partnership with skipper Smith gave them a fine advantage in their bid to retain the Border-Gavaskar Trophy.
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