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The hosts went 2-0 up in the four-Test series by preserving their dominant record in Brisbane - Australia has not lost a Test at the Gabba since 1988 - but it was not all smooth sailing in Smith's captaincy debut.
His first day in charge of the side saw India reach 311-4, but Australia took charge thereafter - building a 97-run first innings lead on the back of a 148-run stand between Smith and Mitchell Johnson.
Smith was named man of the match for his captain's knock of 133, while Johnson's 88 saw the Australian tail wag.
A Johnson-inspired pace attack dismissed India for 224 in the second innings, and despite some nervy moments, Smith's first Test match in charge ended with victory.
Not only was Australia's first day in the field a battle given they picked up just four wickets, each of bowlers Josh Hazlewood, Mitch Starc and Mitch Marsh left the field due to injury and illness.
"I think the way the boys came back from the first day was remarkable. There was that heat stroke, the boys going down like flies so it was a great comeback from that situation," Smith told broadcaster Channel Nine.
"I enjoyed the whole thing [the captaincy].
"Obviously, the first day was one of the toughest days I've probably ever seen in any form of cricket.
"As I said, to come back from there, the way the boys came back on that second morning and bowled beautifully was outstanding.
"To post a big first innings score was crucial for us, and the tail just batted beautifully. We came out and bowled well in the second innings, and created the chances that we needed."
Johnson and opener David Warner were quick to fire barbs at the tourists before the Boxing Day Test in Melbourne, after they tried to unsettle the left-arm quick when he was batting on day three.
"It's all part of the game [sledging]. I love it. The more it comes my way, the better I think. We'll have to see next game what they bring," Johnson said.
Warner, never short of a word himself, also commented on the Indians' tactics, claiming it sparked Johnson's second-innings figures of 4-61.
"Yesterday, a couple of the Indian boys revved up Mitchell Johnson, which is not a good thing and you saw the first spell he bowled today, which was fantastic," the opener said.
Warner also said he would ice his injured thumb over the coming days, in the bid to be fit for Melbourne.
He was hit on the hand batting in the second innings.
"It's very sore at the moment. I'll speak to the medicos and see how I can go. I've got a couple of days off to keep icing it, so I'll see how I go," Warner said.