An ultraviolet-infrared (UV-IR) dual-wavelength photodetector (PD) based on a monolayer (ML) graphene/GaN heterostructure has been successfully fabricated in this work. The ML graphene was synthesized by chemical vapor deposition (CVD) and subsequently transferred onto GaN substrate using polymethylmethacrylate (PMMA). The morphological and optical properties of the as-prepared graphene and GaN were presented. The fabricated PD based on the graphene/GaN heterostructure exhibited excellent rectify behavior by measuring the current–voltage (I–V) characteristics under dark conditions,and the spectral response demonstrated that the device revealed an UV-IR dual-wavelength photoresponse. In addition, the energy band structure and absorption properties of the ML graphene/GaN heterostructure were theoretically investigated based on density functional theory (DFT) to explore the underlying physical mechanism of the two-dimensional (2D)/three-dimensional (3D) hybrid heterostructure PD device. This work paves the way for the development of innovative GaNbased dual-wavelength optoelectronic devices, offering a potential strategy for future applications in the field of advanced photodetection technology.