The Argentine only took over last summer but has failed to land a major trophy following a season blighted by problems off the pitch, including the controversy surrounding Neymar's move to the club, Sandro Rosell's resignation and the tragic passing of former boss Tito Vilanova late last month.
Former Barca midfielder Luis Enrique is the overwhelming favourite to succeed Martino. He resigned as boss of Celta Vigo on Friday and Goal understands he is in pole position to take over at Camp Nou.
Barca's last hope of silverware in 2013/14 disappeared with Saturday's 1-1 draw at home to Atletico Madrid. They went into the final-day contest needing a victory to land the Liga crown on a better head-to-head record than Atleti. All appeared to be going to plan when Alexis Sanchez put them in front in the first half but Diego Godin's towering header at the start of the second denied the hosts.
The reaction from the Blaugrana faithful at the final whistle was telling: applause for Atleti and whistles for the home players and staff.
News of Martino's departure followed soon afterwards with the club's official Twitter feed stating: "Martino has announced that, by mutual agreement with the club, he has ceased being the coach of FC Barcelona."
Martino added at a press conference attended by himself and the club's sporting director Andoni Zubizarreta: "I wanted to say that I have agreed with the club to end my time as Barcelona coach.
"I was proud to coach this club. I admired the players from the outside and then the inside and will keep doing so in what will be a successful future.
"We apologise to the fans for not reaching their expectations. We did not achieve the objectives the club is used to, and has done year after year. We tried until the end but met a rival better than us.
"I want to congratulate Atletico Madrid for their season. They have done very well and deserve their success.
"But above all I want to thank the group of players – to talk of their great qualities as players and as people too."
A sympathetic Zubizarreta added: "I want to thank Tata for his work in what has been a difficult year from the start. He is a great person, good coach and remains a friend.
"We were in Copa final five minutes from the end [before Gareth Bale won it for Real Madrid], and in La Liga until the final seconds.
"We appreciate how he maintained the prestige of the club."
Martino, 51, arrived at Barca having never coached in Europe before but boasted great success in his native South America.
He guided Newell's Old Boys to the Argentine Torneo Final title in 2013 after previously winning the Paraguayan league three times with Libertad and once with Cerro Porteno.
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