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Smith extended his fine recent form with his sixth hundred in 13 matches as Australia racked up 505 in response to India's first-innings total of 408, with the tourists then reduced to 71-1 at stumps in Brisbane.
The hosts looked to be struggled on 247-6 when Mitchell Johnson joined Smith at the crease at the Gabba, but the duo put on a crucial 148-run partnership before Mitchell Starc (52), Nathan Lyon (23) and Josh Hazlewood (32 not out) added useful contributions.
Smith was eventually dismissed for 133 in his first Test since being appointed as stand-in captain in the absence of the injured Michael Clarke, while Johnson plundered 88 from 93 balls.
"Mitchell Johnson came out and really took it to the Indian bowlers," said Smith. "He took them on and played some terrific cricket.
"To be fair, our whole tail battled beautifully. Both Mitchs batted outstanding and Nathan Lyon and Josh Hazlewood on debut were also very good as well.
"To get us up over 500 with a lead of 90-odd was remarkable and put us in a good position.
"We had a good day of cricket there at the end and hopefully we start well in the morning and can pick up a few wickets."
Smith feels he produced a captain's innings on Friday.
He added: "I said before the Test match that I wanted to lead from the front with my performances so hopefully I've done that this game and hopefully it continues for me as well.
"I've really enjoyed the last couple of days - the boys have really supported me really well."