Laser-induced ultrafast photovoltaie effect is observed in LaSrA104 single crystal at ambient temperature withoutany applied bias. An open-circuit photovoltage is obtained when the wafer is irradiated by a 248-nm-KrF laser pulseof 20 as duration. The response time and full width at half maximum of the photovoltage pulse are 6 as and 19 ns,respectively, indicating that LaSrAlO4 single crystal has potential application in ultraviolet detector.