The World Cup 1994-winner thinks the Barcelona star, who shone for Brazil before injury last summer, will break the legendary striker's 77-goal tally for his country.
Romario believes Pele's long-standing goal record for Brazil will be broken by Barcelona forward Neymar.
The former Santos star was arguably the star player at last summer's World Cup until injury ruled him out of the Selecao's semi-final against Germany – a game they lost 7-1.
Having racked up 42 goals in 60 caps for Brazil, Neymar is fifth in the nation's all-time goalscorer list behind Pele (77), Ronaldo (62), Romario (55) and Zico (48).
Att the age of 23, he could yet play in at least another two World Cups and Romario is convinced he will eventually become the greatest goalscorer in his nation's history.
“I think because of his age – though he still has others to topple – Neymar will become to top goalscorer in Brazil's history, surpassing Pele,” the former PSV and Barca forward told Folha de Sao Paulo.
“It wouldn't hurt if Neymar leapfrogged me in the list. I left my mark on history and now it's his turn.”
Neymar overtook Romario's tally of 39 strikes as a Barcelona player earlier this month when he scored his 40th goal for the club, while he has found the back of the net 26 times in 34 games this season.
Neymar is Brazil's only genuine star after admitting his nation no longer boast the array of attacking talent they once had.
The Selecao boss, 51, won the World Cup in 1994 as part of a squad that featured the likes of Romario and a 17-year-old Ronaldo.
However, at last summer's tournament, where Brazil crashed out to Germany 7-1 in the semi-finals, Fred led the line with Neymar and Oscar operating in wider roles.
And Dunga has admitted the Barcelona star is an increasingly rare talent, with the country failing to produce the quality for which they were once famed.
"What is happening in Brazilian football is that we used to have players who scored a lot of goals in Europe and who were points of references, but we no longer have players like that nowadays," Dunga told SportTV.
"We used to have players like Careca, Ronaldo and Rivaldo, but countries like Portugal and Holland now produce those kinds of players.
"We do not have any players who are really making waves. We only have Neymar at the moment.
"This is very worrying for Brazilian football. We need to have patience, though, and remain calm."
Dunga was appointed Luiz Felipe Scolari's replacement after their shock World Cup exit and he immediately named Neymar as his captain, who took the armband from Thiago Silva.
The 23-year-old has been in fine form for the La Liga leaders this season, netting 26 goals in 34 appearances in all competitions.
