Sprinter Cal, who carried the Spanish flag at the opening ceremony for the 2008 Beijing Olympics, competed in the C1 class where the competitor kneels in his craft and uses a single paddle.
He won silver and gold in Athens in 2004, two silvers in Beijing and another silver in London in 2012.
"Spain's most decorated Olympian is retiring," COE said on their Twitter feed. "Just one word for our champion @DavidCal1: thank you!"
Spanish media reported Cal had decided to retire because he had lost his motivation, partly due to problems in securing funding.
He was raised in one of the small coastal villages near Pontevedra in north-west Spain and started canoeing aged eight.
"I lived near the beach," he said in an interview with Reuters shortly before the London Games.
"I simply saw the people out there, it caught my attention. One day with a friend we had a go. I tried it, enjoyed it and there we are."
(Reporting by Iain Rogers, editing by Justin Palmer)
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