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Based on (2712.4 ± 14.3) × 106ψ(3686) events collected at the BESIII detector operating at the BEPCII collider, we present the first observation of the decay ψ3686→K−Λ1520Ξ¯+ + c.c. The product branching fraction Bψ3686→K−Λ1520Ξ¯++c.c.×BΛ1520→pK− is measured to be (9.47 ± 0.75 ± 0.97) × 10−7, where the first uncertainty is statistical and the second systematic.