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The modification by molybdenum trioxide (MoO₃) buffer layer on the electronic structure between Co and black phosphorus (BP) was investigated with ultraviolet photoemission spectroscopy (UPS) and X-ray photoemission spectroscopy (XPS). It was found that the MoO₃ buffer layer could effectively prevent the destruction of the outermost BP lattice during the Co deposition, with the symmetry of the lattice remaining maintained. There is a noticeable interfacial charge transfer in addition to the chemical reaction between Co and MoO₃. The growth pattern of Co deposited onto the MoO₃/BP film is the island growth mode. The observations reveal the significance of a MoO₃ buffer layer on the electronic structure between Co and black phosphorus and provide help for the design of high-performance Co/BP-based spintronic devices.