Mold fouling can degrade the physical properties and reduce the aesthetic value of the molded product. A plethora of research efforts have tried addressing these drawbacks, however, an effective method to prevent the foregoing adverse effects of mold fouling is still a challenge. Here, the fouling performance of aluminum alloy with a nanocrystalline surface layer fabricated by High Pressure Shot Peening (HPSP) during vulcanization has been investigated. Results indicate that an HPSP-treated sample shows excellent resistance of mold fouling with only 1/8 weight gain after 25 cycles, compared to its HPSP-free counterpart. The improved release performance can be attributed to the compact passivation layer with a larger thickness and low-energy surface obtained after HPSP treatment, as well as the strengthened surface with a lower friction coefficient.