A novel yet simple approach to fabricate and pattern wrinkled surfaces on polymers is presented. Only by irradiating an electron beam onto a polymer, wrinkles are created on the polymer surface. Electron irradiation produces a bilayer polymeric structure comprising a degrading upper layer and a pristine bottom layer. Electron irradiation also increases the polymer surface temperature to a point much higher than the glass-transition temperature of the upper layer, leading to drastic thermal expansion of the upper layer. As a result, significant compressive force is applied to form surface wrinkles. The mechanism behind the wrinkle formation and the effects of electron irradiation parameters on the wrinkle characteristics are discussed. In addition, by this electron irradiation approach, a patterned wrinkle structure is uniquely prepared.