Put in to bat, Australia lost the opening duo of Matt Renshaw (11) and David Warner (25) early but Smith (107 retired) and Marsh (104 retired) put on 156 runs for the third wicket to deny the home boys any more inroads into the game.
Promising Haryana medium pacer Navdeep Saini, who came in as a first change bowler, accounted for the early wickets of Renshaw and then Warner, whose quickfire 30-ball knock contained four boundaries.
But Smith and Marsh started off on a positive note leaving the early setbacks behind and went after the loose deliveries from the India A bowlers.
Resuming the post-lunch session at 81/2, the right-handed duo added 130 runs in 33 overs without losing any more wickets to help Australia reach 211/2 at tea.
In due course, Smith, who has 17 hundreds in 50 Tests, also brought up his 30th first class ton in his 100th game.
Smith, who consumed 161 deliveries for his knock, hit 12 boundaries and a six while Marsh's innings was the more subdued which came from 173 balls and contained 11 hits to the fence and one over it, as the duo took the score to 211/2 before Smith walked off.
Thereafter, Peter Handscomb (45) joined Marsh and the duo added 79 runs for the fourth wicket before Marsh too joined his skipper in the dressing room after reaching the three-figure mark.
With both the centurions back in the pavilion, the India A bowlers sniffed the chance of a comeback and skipper Hardik Pandya responded well by dismissing Handscomb to leave the visitors at 305/5.
All-rounder Mitchell Marsh (16 not out) and wicketkeeper-batsman Matthew Wade (7 not out) then spent some quality time in the middle as the day came to an end with the visitors at 327/5.
For the hosts, Saini returned with figures of 2/27 from his 12.4 overs while Pandya chipped in with one wicket as the rest of the bowlers failed to impress on a wicket which had a tinge of grass and offered good bounce.
Brief Scores: Australia 1st innings: 327/5 (Steve Smith 107 retd, Shaun Marsh 104 retd, Peter Handscomb 45, David Warner 25, Navdeep Saini 2/27) vs India A.
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