Zagallo, who led Brazil to World Cup victory in 1970 and the runners-up spot in 1998, told reporters he will run for a vacant vice-presidency in the Brazilian Football Confederation (CBF).
He is expected to face opposition from Marco Polo Del Nero, who recently joined FIFA's executive committee.
"You know me, I wasn't going to rest on my laurels," said Zagallo, who would be one of five CBF vice-presidents, each representing a region of the country, if elected.
"I'm going to learn about the bureaucratic aspects but I will really be thinking about the Brazilian national team.
"It would be my last World Cup," he added, referring to the 2014 tournament which Brazil will host.
"This is my last chance to take Brazil to a sixth world title. I will help out with the experience I have."
Zagallo was involved with four of Brazil's World Cup triumphs. He played in the 1958 and 1962 teams, was coach in 1970 and worked as assistant to Carlos Alberto Parreira in 1994.
Zagallo's nomination for the south-eastern region vice-presidency, has opened up an internal battle in Brazilian football.
He was put forward by the Rio de Janeiro football federation while Sao Paulo is expected to nominate Del Nero.
The position was left vacant when Jose Maria Marin took over the CBF presidency following the resignation of Ricardo Teixeira, who quit citing health reasons although he also faced corruption allegations.
Marin could continue until the end of Teixeira's mandate in 2015, though there is speculation that he could leave before then which would leave Zagallo with a chance of taking over the CBF presidency.