Boro reached an agreement with the 35-year-old former Barcelona and Manchester United shot-stopper to cancel the second year of his contract.
Valdes started 28 league games last season and Brad Guzan, who is also leaving the club for Major League Soccer side Atlanta United, featured in the other 10 games.
Greece international Dimi Konstantopoulos, who made one appearance last season, is now the only goalkeeping option in the senior squad as Boro prepare for the Championship next season.
(Reporting by Hardik Vyas in Bengaluru, editing by Ed Osmond)
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