Busquets, who served as Spain's World Cup captain, was one of three players to miss a penalty as Luis Enrique's team lost to Morocco 3-0 in a shootout after a scoreless regulation match.
The 34-year-old was a member of Spain's winning teams at the 2010 World Cup and the 2012 Euros, making it three straight major tournament victories for the country.
Busquets, the lone member of Spain's 2010 World Cup winning team to play in Qatar, has announced the end of his nearly 15-year international career.
'It has been an honor to represent my country and take it to the top, to be a World and European champion, to be captain and to play so many games with greater or lesser success,' Busquets wrote in a lengthy Instagram post.
'But always giving everything and contributing my grain of sand so that everything was the right way as possible and that everyone felt how important they are, helping everyone and fighting for the same goal, with unique, unforgettable and historical experiences.'
Following Spain's early World Cup defeat, Luis Enrique was fired as manager a few days before Busquets announced his retirement.
Busquets made his debut for Spain against Turkey in 2009 and went on to play 143 times for the country.
Vicente del Bosque's 2010 World Cup-winning team defeated the Netherlands 1-0 in extra time to win the trophy for the first time, and he participated in every game.
'I would like to thank all the people who have accompanied me on this long journey,' Busquets added on his Instagram page.
'From Vicente del Bosque who gave me the opportunity to start, to Luis Enrique for making me enjoy until the last second. I also thank Julen Lopetegui, Fernando Hierro and Robert Moreno for their trust, as well as all of his staff.
'And of course to each and every one of my teammates, with whom I have struggled to try to take the team where it deserved, with more or less success but always giving everything and with the greatest of pride.'
Busquets was included in the team of the competition as Spain defended their title as European Champions in 2012 by defeating Italy 4-0.
Against Macedonia and Belarus in Euro 2016 qualification, he scored just twice for Spain.
Busquets will represent Spain on the field in the World Cup in Qatar and the 2020 Euros under Luis Enrique's leadership.
'To all the followers, for the daily support received and especially when things did not turn out as we expected. That is when you are most needed and most united you have to be.
'And of course, most importantly, my family. For supporting me at all times and in all my decisions and sharing this path while being away for many days and making me always feel close so that I could give my best.'
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