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An ultraviolet sensitive ultrafast photovoltaic effect is observed in tilted 10° KTaO3 (KT) single crystals. The rise time of the transient photovoltaic pulse is 497.4 ps and the full width at half maximum is 974.6 ps under irradiation of a 266 nm laser pulse with 25 ps duration. An open-circuit photovoltage sensitivity of 328 mV/mJ and a photocurrent sensitivity of 460 mA/mJ are obtained. The experimental results demonstrate the potential applications of KT single crystals in ultraviolet detection.