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A strong demand currently exists for ferromagnetic (FM) materials with adjustable magnetic properties. In this study, using laser illumination, we demonstrated the direct and efficient modulation of the magnetism of thin FM films covered by all-inorganic cesium lead bromide (CsPbBr 3 ) perovskite quantum dots (QDs). The surface morphology and characteristic sizes of the CsPbBr 3 QDs changed considerably and evolved gradually with the increase in the laser illumination time, triggering a series of redox and interfacial diffusion processes, particularly at the interface of the CsPbBr 3 QDs/Co heterostructure. The magnetic properties were thus adjustable by varying the magnetic hysteresis loop in accordance with the Co thin film thickness. We believe that this study will pave the way for advanced spintronic applications.