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Some cyanide‐bridged complexes are known for exhibiting slow magnetic relaxation behavior in a light‐induced metastable state. Herein, an unexpected reverse effect is observed for the first time in the S=1/2 {FeIILS‐CoIIILS‐FeIIILS} (HS=high spin, LS=low spin) ground state of a novel V‐shaped trinuclear cyanide‐bridged {Fe2Co} complex. In this complex, light‐switchable iron‐cobalt charge transfer with repeatable off/on switching of slow magnetic relaxation is discovered upon alternating laser irradiation at 785 and 560 nm. An important characteristic of the present compound is that the S=1/2 ground state exhibits slow magnetic relaxation before irradiation, whereas this is accelerated after irradiation. This is different from the typical behavior, where the light‐induced metastable state exhibits slow magnetic relaxation. [ABSTRACT FROM AUTHOR]