Smith, who was not dismissed by India in last week's Adelaide Test win with scores of 162 and 52, continued to be the bane of the tourists with another defiant knock. He has scored 279 so far in the series.
His intuitive stroke-making was again a delight and he danced down the wicket to club spinner Ravichandran Ashwin for two sixes over long-on in one over.
At the close, with a fierce storm about to break, Australia were 221-4 in reply to India's 408, with Smith unbeaten on 65 and Mitchell Marsh on seven.
“It's not about Steve Smith or any names that we want to take out here, it's going to be a couple of wickets that we want to take tomorrow morning,” said Ashwin. “I think we are in front of the game at this point of time. Our 400 is enough if we can get a couple of wickets tomorrow morning.”
Earlier in the day, debutant Josh Hazlewood captured five wickets and Brad Haddin equalled a wicketkeeping record as Australia dismissed India for 408 at lunch.
Paceman Hazlewood led the way with three scalps in the second morning as the Australians bounced back after Wednesday's horror show in the field in sweltering conditions.
"Yesterday was a pretty tough slog out in the heat," said Hazlewood. "It wasn't much cooler today but we all came out well and bowled to our plans and picked up the last six wickets for about where we wanted them."
Like Sports on Facebook, follow @ETribuneSports on Twitter to stay informed and join in the conversation.
COMMENTS
Comments are moderated and generally will be posted if they are on-topic and not abusive.
For more information, please see our Comments FAQ