The 35-year-old defender has enjoyed an extremely successful career with the Catalan club, winning six La Liga titles and three UEFA Champions League crowns in his time at Camp Nou.
However, the centre-back, who has also won the UEFA European Championship and the FIFA World Cup for Spain, has been plagued by injury problems in recent years.
Puyol twice underwent surgery to resolve a knee problem last year, finally returning to action in October following a lengthy spell on the sidelines.
But Puyol admits the surgeries have taken a toll on his performances for Barca and revealed that the club will rescind his contract at the end of the current campaign.
The Camp Nou captain called a short press conference on Tuesday to announce the news.
He said: "The motive for this press conference is to inform you that I will leave FC Barcelona at this end of the current season.
"The club knows of my decision. It doesn't mean that I am leaving today, there are three months of the season left to play.
"I am tired after so many injury problems and operations. The club will rescind my contract."
Puyol has been restricted to 12 appearances for Barca this season, although he did find the net last Sunday in the 4-1 win over Almeria and in a 5-1 Copa del Rey triumph against Levante in late January.
He is the second big-name Barca player to announce he will leave Camp Nou at the end of the season, with goalkeeper Victor Valdes also set to depart.
