Smith looked at ease on a true pitch, smashing his way to an unbeaten 72 off 101 balls. The captain added 121 runs for the unbroken second wicket with David Warner (54), who was dropped in the very first ball of the match by Karun Nair off Bhuvneshwar Kumar.
Smith's innings had 10 boundaries while Warner hit eight fours and a six.
Ajinkya Rahane, leading the side in place of an injured Virat Kohli, could hardly do anything after Ishant Sharma's replacement Bhuvneshwar bowled a terrible first spell.
To make matters worse, his premier spinner Ravichandran Ashwin could hardly trouble the Australia captain even though he got bounce off the wicket.
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With ball coming onto the bat nicely, Smith played the role of an enforcer to perfection while Warner played the second fiddle well after initial period of struggle. It was a different kind of batting from the dashing left-hander but it was effective enough to get to his first half-century of the series.
The pitch was exactly to Australia's liking with Smith winning a good toss. But Bhuvneshwar, perhaps buoyed by the bounce, bowled short to both the batsmen who played the cut shot at will.
Smith started with a few drives off Umesh and then warmed up to Bhuvneshwar, who completely erred in length. Bhuvneshwar was hit for six boundaries in his eight overs.
The only bowler who looked like causing some trouble was Ravindra Jadeja as he beat Smith's bat a couple of times by virtue of being quicker through the air and off the pitch.