"Certainly it's a big series for us. We've had a lot of great contests over the years. South Africa got the better of us at home so we'd love to get them back for that one," said Smith ahead of the start of the first Test at Kingsmead in Durban on Thursday.
South Africa won 2-1 in a three-Test series in Australia in November 2016, their third straight series win there.
However, Australia have a brilliant record away in South Africa, and it is an anomaly that Smith and his opposite number Faf Du Plessis put down to the similar conditions in both countries.
Australia are aiming to build on a "magnificent" home summer which included a 4-0 Ashes defeat of England.
"The conditions are similar but it's still an away tour for us. I've got a goal as captain to play really well away from home and start winning series, so this is a really good opportunity for us," said Smith.
The world's leading Test batsman, Smith said a century in tough conditions at Centurion on Australia's previous tour in 2013/14 had given him the confidence that he could score runs against any bowling attack.
Du Plessis is fully aware of Smith's threat having played alongside him in the Indian Premier League, and he is hoping to use that experience to bring about his rival's downfall.
"The last series we played against him he was their best batter but to some degree we did keep him quiet," he said.
"He's obviously a very good player but it's similar to what I said about the Indian team. They have one or two star batsmen. If you can put pressure on them and keep them quiet it obviously reflects how the series will go."
Du Plessis said no pressure had been put on groundsmen to prepare pitches to help the South Africans following the controversy that marred the recent series win over India.
"I think I learned my lesson from that," he said.
"Australia and South Africa are very similar teams and they play in similar conditions. We'll play on what we get. We've asked for nothing."
It seems likely that South Africa will switch from the policy of four specialist fast bowlers that was used against India, with an extra batsman likely to be picked.
With Temba Bavuma not fully recovered from a finger injury, Theunis de Bruyn is a strong candidate, especially as he can bowl a few overs of seam to back up the main bowlers.
Injuries and lack of form have plagued the South Africans recently. Du Plessis will play, though, despite having broken his right index finger less than a month ago.
"I've played with finger injuries before," he said. "The biggest battle you have to get over is the mental side of things. I have had three good nets, hitting a lot of balls, but the biggest thing is mentally to be ready for the battle and I'm ready for that."
First Published: February 28, 2018, 8:01 PM IST