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The 50-year-old's future has been a hot topic since last year's Women's Women World Cup on home soil after he was linked with the Swedish men's side and the US women's national team.
Gustavsson opted to see out the final year of his deal with Australia and in a cruel twist of fate it was the US who all-but ended the Matildas' Olympics medal hopes in the early hours of Thursday morning by sealing a 2-1 win.
After three underwhelming performances saw them crash out at the group stage for the first time since 2000, the Matildas' Olympic campaign must be a reality check for the Australian game.
Australia clung to hope it could squeak through to the quarterfinals in France as a best third-place finisher, but results from other groups went against them.
Gustavsson led the Matildas to fourth-placed finishes in both the Tokyo Olympics and last year's World Cup, but has been criticised more recently over tactics and team selection alike.
FA's decision to move quickly has been done with a view to attracting the highest-calibre candidate, although the most-likely homegrown contender — former Melbourne Victory coach Joe Montemurro — has recently signed a deal with French club Lyon.
FA will hope that hosting the 2026 Asian Cup will also strengthen its chances of attracting a top-tier coach.
Gustavsson informed his players of his departure in the aftermath of the loss to the USA.
"Australian football will be forever in my heart, and I will be watching on and cheering on your success in the future," Gustavsson said in a statement.
"This journey with the team has had many incredible moments and memories that I will forever treasure."
His exit marks the end of a period where the women's game in Australia has undergone an explosion in popularity.
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Gustavsson deserves credit for turning Clare Hunt, Cortnee Vine and Kyra-Cooney Cross into mainstays of the Matildas set-up and backing Mackenzie Arnold as his first-choice goalkeeper.
Those success stories are tempered with concerns over his over-reliance on Australia's golden generation, his inability to broaden the team's depth, and the fact the Matildas have struggled to develop a discernible style to match it with the world's best.
Gustavsson took over the Matildas' management in September 2020, having worked as an assistant with the United States' national team on two occasions throughout a 21-year coaching career in Sweden.
He did not relocate to Australia during his tenure as Matildas boss and it is yet to be seen if FA will make that a prerequisite for any of his prospective replacements.
"As part of our commitment to continuous improvement, we will conduct a thorough review of the campaign, as we do with all our national teams following the conclusion of tournaments and each cycle," said FA chief executive, James Johnson.
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