The practical application of perovskite oxides as electrocatalysts for oxygen evolution reaction (OER) has been greatly hindered by their limited catalytically active sites and poor electrical conductivity. Herein, we report the use of a perovskite-oxide nanofilm as highly improved electrocatalyst for OER. A facile fabrication method, pulsed laser deposition (PLD), is employed for the first time to fabricate the SrCo0.85Fe0.1P0.05O3−δ nanofilm on nickel foam (SCFP-NF) with abundant active sites and enhanced electrical conductivity. We find that the SCFP-NF fabricated by PLD exhibits excellent OER activity and durability in alkaline solutions. Especially, the PLD method can create a large amount of oxygen vacancies on the surface of the perovskite nanofilm, leading to a high concentration of highly oxidative oxygen O22−/O−. This O22−/O− species is generally recognized to be active for OER. As a result, the SCFP-NF catalyst with low mass loading (≈30 μg cm-2) demonstrates a remarkable OER activity with a low overpotential of 290 mV and a superb stability up to 200 h at 10 mA cm−2 in alkaline media. The catalytic performance of this perovskite nanofilm is superior to most of the reported metal-oxide-based catalysts and benchmark RuO2. Our findings show that the catalytic performance of oxide-based electrocatalysts can be greatly improved by defect-engineering, and the PLD and other film fabrication methods may help us to realize practical application.