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In this study, we successfully fabricated nanocrystal ZnO doped Cr3+ by solgel method. Crystalline structure, morphology, and optical characteristics such as optical bandgap, and emission were researched by X-ray differactometer, transmission electron spectroscopy, UV-vis absorption, and photoluminescence measurements. X-ray differaction patterns showed no other secondary phase in doped ZnO samples. They were in wurtzite phase and lattice constant (c) was decreased when the Cr3+ content increased. When increasing Cr3+ content in ZnO, the intensity of photoluminescence emission was reduced which was indicated that the reduction of radiative recombination rate because of the formation of heterojunction between ion Cr and ZnO. As a result, photocatalytic activity by MB degradation under natural visible light showed the enhancement of Cr3+ doped ZnO samples in comparison to the pure ZnO.