Popovic, capped 59 times by Australia in a 12-year international career, said he would no longer turn out as a player for Sydney FC but would take up a position as assistant coach with the same club.
"It was a pretty easy decision for me," Popovic told a news conference.
"As an athlete you just know when the time is right and when you are not getting out of yourself what you can. You want to do it but it is just not there anymore."
The 35-year-old defender was a key member of the Australian national team for more than a decade, helping the Socceroos end a 32-year World Cup drought by qualifying for the 2006 tournament in Germany.
Popovic also spent five years with English club Crystal Palace as well as overseas stints in Japan and Qatar.
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