The interplay between light and magnetism sparks groundbreaking concepts for the next-generation versatile spintronic and nanoelectronic devices. However, direct measurements of light-magnetism coupling remain challenging due to the intrinsic difficulties in characterizing these properties simultaneously. Herein, via harnessing magnetic proximity and anomalous Hall effect (AHE), we report the effective modification of magnetism in the graphene/CrSBr heterostructure by an unpolarized 405 nm light. The emergence of magnetism in graphene is ascribed to the proximity effect, which arises from its coupling with the neighboring CrSBr. The photoinduced charge transfer doping into graphene exerts a precise tune over the Fermi level (), facilitating the optical control of carrier density and mobility. This operation engenders an adjustable anomalous Hall resistance and magnetoresistance congruent with the Fermi level tuning, further verified by surface potential measurements. In parallel, high-performance magneto-photoresponse has been realized, which is believed to result from spin polarization-enhanced photoinduced charge separation. Our study offers insights into the interplay between light and magnetism, showcasing the potential of 2D proximity-coupled heterostructures in opto-spintronics.
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