Luiz Felipe Scolari, 65, won the 2002 World Cup but the hosts could only finish fourth at this year’s event.
Brazil was thrashed 7-1 by Germany in the semi-finals, their joint-heaviest loss ever and first home competitive defeat for 39 years.
They then lost 3-0 to the Netherlands in the play-off for third place.
Luiz Felipe Scolari’s contract was set to expire after the tournament but Globo TV says his resignation will be confirmed on Monday by the CBF, Brazil’s football federation.
UOL News, a Brazilian website, is also reporting that Luiz Felipe Scolari has quit, quoting two CBF sources.
During the defeat by the Netherlands, Luiz Felipe Scolari, in his second spell in charge of the national team, was booed every time his image appeared on the big screen inside the stadium in Brasilia.
Luiz Felipe Scolari first took over the Brazil side in 2001 and guided them to World Cup success a year later, beating Germany 2-0 in the 2002 final in Yokohama, Japan.
After spells in charge of Portugal, Premier League side Chelsea, Bunyodkor of Uzbekistan and Brazilian club Palmeiras, he resumed control of the national team in 2012.
Brazil hosted and won the Confederations Cup in 2013, beating Spain 3-0 in the final, and wa favorite to win a sixth World Cup.
They finished top of their group after two wins and a draw from their three matches, before edging past Chile on penalties in the last 16.
They beat Colombia 2-1 in the quarter-finals, but lost top goalscorer Neymar to a spine injury and captain Thiago Silva to suspension.
In the semi-final, Brazil were 5-0 down to Joachim Low’s Germany after only 29 minutes, before losing 7-1.
Luiz Felipe Scolari described the defeat as “the worst day of his life” and asked for forgiveness from the Brazilian people.
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