Few‐layered antimonene (FLSb) nanosheets were noncovalently functionalized with fullerene C60 clusters by quick addition of a poor solvent (i.e., acetonitrile) into a mixed dispersion of FLSb and C60 in a good solvent (i.e., toluene). In a flash‐photolysis time‐resolved microwave conductivity (FP‐TRMC) measurement, the FLSb‐C60 composite, (FLSb+C60)m, showed a rapid rise in transient conductivity, whereas no conductivity signal was observed in the single components, FLSb and C60. This demonstrated the occurrence of photoinduced charge separation between FLSb and C60 in (FLSb+C60)m. Furthermore, a photoelectrochemical device with an electrophoretically deposited (FLSb+C60)m film exhibited an enhanced efficiency of photocurrent generation, compared to those of the single‐components, FLSb and C60, due to the photoinduced charge separation between FLSb and C60. This work provides a promising approach for fabrication of antimonene–organic molecule composites and paves the way for their application in optoelectronics.