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The field of photovoltaics is revolutionized in recent years by the development of two-dimensional (2D) type-II heterostructures. These heterostructures are made up of two different materials with different electronic properties, which allows for the capture of a broader spectrum of solar energy than traditional photovoltaic devices. In this study, the potential of vanadium (V)-doped WS 2 is investigated, hereafter labeled V-WS 2 , in combination with air-stable Bi 2 O 2 Se for use in high-performance photovoltaic devices. Various techniques are used to confirm the charge transfer of these heterostructures, including photoluminescence (PL) and Raman spectroscopy, along with Kelvin probe force microscopy (KPFM). The results show that the PL is quenched by 40%, 95%, and 97% for WS 2 /Bi 2 O 2 Se, 0.4 at.% V-WS 2 /Bi 2 O 2 Se, and 2 at.% V-WS 2 /Bi 2 O 2 Se, respectively, indicating a superior charge transfer in V-WS 2 /Bi 2 O 2 Se compared to pristine WS 2 /Bi 2 O 2 Se. The exciton binding energies for WS 2 /Bi 2 O 2 Se, 0.4 at.% V-WS 2 /Bi 2 O 2 Se and 2 at.% V-WS 2 /Bi 2 O 2 Se heterostructures are estimated to be ≈130, 100, and 80 meV, respectively, which is much lower than that for monolayer WS 2 . These findings confirm that by incorporating V-doped WS 2 , charge transfer in WS 2 /Bi 2 O 2 Se heterostructures can be tuned, providing a novel light-harvesting technique for the development of the next generation of photovoltaic devices based on V-doped transition metal dichalcogenides (TMDCs)/Bi 2 O 2 Se., (© 2023 The Authors. Small published by Wiley-VCH GmbH.)