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We report on the fabrication of γ-phase copper iodide (γ-CuI) and beta-gallium oxide (β-Ga2O3) heterostructure device and obtaining the ultraviolet (UV) radiation responsive photovoltaic action. The crystalline γ-CuI with predominant (1 1 1) plane orientation was deposited on the β-Ga2O3 by thermal evaporation process under vacuum condition. The electrical analysis revealed that the γ-CuI/β‐Ga2O3 heterojunction possess an excellent rectifying diode characteristic with high rectification ratio and turn-on voltage. The fabricated heterojunction device showed a photovoltaic action under solar-blind UV irradiation (254 nm) with outstanding photovoltage of 0.706 V and photocurrent of 2.49 mA/W. The device also showed a photovoltaic action under illumination of 365 nm and 300–400 nm wavelength of UV light, corresponding to absorption due to the γ-CuI layer. The UV irradiation-induced photovoltaic action in the γ-CuI/β‐Ga2O3 with outstanding photovoltage and excellent diode characteristics can be significant for self-powered UV photodetector applications.