But he never got to take a spot kick in the shootout that Croatia won 4-2 to move into the semi-finals.
Pre-tournament favourites Brazil must now wait at least another four years to win their sixth World Cup — their last dates back to 2002.
“I am psychologically destroyed. It is definitely the defeat which has hurt me the most, which left me paralysed for ten minutes after the match, after which I burst into tears without being able to stop,” Neymar said in an Instagram message.
“It is going to hurt for a very long time, unfortunately,” he added.
Neymar said immediately after Brazil crashed out that he might have played his last match for his country — but Pele urged him to “keep inspiring us.”
The 82-year-old said on Instagram he hoped the superstar forward would carry on playing, adding that goalscoring achievements were no match for the honour of representing Brazil.
“You know, as I do, that no number is greater than the joy of representing our country,” Pele wrote.
“I’m 82 years old, and after all this time, I hope I’ve inspired you in some way to get this far…. Your legacy is far from over.
“Keep inspiring us. I will continue punching the air with happiness with every goal you score, as I have done in every game I’ve seen you on the pitch.”
Pele, who was hospitalised earlier this month during treatment for colon cancer, congratulated Neymar for equalling his goalscoring record.
“I learned that the more time passes, the more our legacy grows,” Pele wrote.
“My record was set almost 50 years ago, and no one has been able to get close to it until now. You made it, my boy. That adds to the greatness of your achievement.”