The Barcelona forward was named captain by former coach Dunga when the latter took charge of the Selecao for a second time after the 2014 World Cup, reports Xinhua.
But Alberto said Tite feels that it is time for a change. Tite replaced Dunga as the national team coach earlier this week after Brazil's group-stage elimination from the ongoing centenary edition of the Copa America.
"If I was the national coach, the first thing I would do would be to ask Neymar to have the humility to return the captain's armband so the coach can choose another player," Carlos Alberto was quoted as saying by the Sambafoot news portal. "It does not suit him to be captain.
"Pele was never captain. Neither was Garrincha, or Ronaldo, Rivaldo or Nilton Santos. Why does Neymar have to be captain of the national team?"
Neymar, who missed the Copa America after Barcelona refused to release him for the tournament in the US, has been criticized for his recent international performances, which have been marked by ill-discipline and a lack of goals.
The 24-year-old was replaced as captain during the continental tournament by Inter Milan center-back Miranda.
"It would be better to let him play and free him from the responsibility of leading the group," Alberto said. "Leave him free to just think about playing football. He would do more for the team than he has done. I would leave Miranda as captain."
Alberto added that the captain should be decided by both the national coach and Brazil's football confederation.