Neymar turned his R$7,000 ($2,534) entry stake into R$79,440 ($28,758) before being eliminated in the final of the High Roller event, organisers said.
"I'm very happy to be playing this tournament for the first time and for reaching the final with some great players," the 26-year old Paris St Germain forward said.
"This is a new experience for me."
Neymar signed up for the tournament with five of his friends on Monday and was the only one of the six to make it through to the second day.
The final table of nine players was scheduled to play on Wednesday night (AEST) but the contestants agreed to postpone for a day to allow Neymar to attend a friend's wedding.
He returned to compete on Thursday but after almost four hours of play was eliminated after betting big on two consecutive losing hands.
Brazilian legend Ronaldo is also a keen poker player and spokesman for an online poker company, while Manchester City's Gabriel Jesus and former Paris Saint-Germain striker Nene also competed in Brazilian Series of Poker competitions this week, a spokesman told Reuters.