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Cube-like Cu2MoS4 nanoparticles with low-index facets and high crystallinity were fabricated via a hydrothermal method. The as-obtained nanocubes with an average size of 40-60 nm are composed of stacking-Cu2MoS4 layers separated by a weak Van der Waals gap of 0.5 nm. A strong absorption at visible light region is observed in the nanocube aqueous solution, indicating its optical-band gap of 1.78 eV. The photocatalytic measurements reveal that the nanocubes can thoroughly induce the degradation of methyl orange under visible light irradiation with good structural stability. Our finding may provide a way in design and fabrication of transition metal dichalcogenide nanostructures for practical applications.