Herein, a series of g-C3N4 modified Bi2MoO6 nanocomposites using Bi2MoO6 and melamine as original materials are fabricated via sintering process. For presynthesis of Bi2MoO6 an ultrasonic-assisted hydrothermal technique is researched. The structure and composition of the nanocomposites are characterized by Raman spectroscopy, X-ray diffraction (XRD), and high-resolution field emission scanning electron microscopy (SEM). The improved photoelectrochemical properties are studied by photocurrent density, EIS, and amperometric i-t curve analysis. It is found that the structure of Bi2MoO6 nanoparticles remains intact, with good dispersion status. The as-prepared g-C3N4/Bi2MoO6 nanocomposites (BMC 5-9) are selected and investigated by SEM analysis, which inhibits special morphology consisting of Bi2MoO6 nanoparticles and some g-C3N4 nanosheets. The introduction of small sized g-C3N4 nanosheets in sample BMC 9 is effective to improve the charge separation and transfer efficiency, resulting in enhancing of the photoelectric behavior of Bi2MoO6. The improved photoelectronic behavior of g-C3N4/Bi2MoO6 may be attributed to enhanced charge separation efficiency, photocurrent stability, and fast electron transport pathways for some energy applications.