The 2022 British Open champion tied for 10th at the Tokyo Olympics three years ago but, as world number 62, he has four other Australians ahead of him in the world rankings, which will determine which two players go to Paris.
Smith's defection to the LIV Tour means he earns no rankings points from most of his events so doing well at Augusta as well as May's PGA Championship and the U.S. Open in June is essential if he is to play at Le Golf National from August 1-4.
"It's desperately a place that I want to get to and represent Australia," the former world number two told reporters from Florida on Tuesday.
"I have to play well to get there, I know I have to play well, and I'm probably only going to get three or four shots at it before they make the selection. I guess it is more pressure."
Smith has finished in the top five at Augusta three times in seven visits and getting his hands on the famous green jacket remains another major ambition.
"It's just such a cool place ... I desperately want to get it and it would be awesome if I did," he added.
"We've just had three weeks off and I've been out on the course focusing on shot-shaping and controlling flight, which I think is pretty crucial for playing good around there."
The 30-year-old is getting used to having more time off with the much-touted unification between LIV and the U.S. PGA Tour still looking a long way off.
Smith is not complaining.
"I've probably got another four or five weeks off every year in the last couple of years and been able to spend more time in Australia," he said.
"I don't know if I'm willing to sacrifice being away from my family and stuff as much as I had in the past."
Smith's team posted a picture on social media of him shorn of his mullet on Monday but it turned out to be an April Fool's prank and the famous hairstyle will be on show at the LIV event in Adelaide later this month.
"It was probably a unanimous decision on the whole tour that that was the best event that we had (last year)," he said.
