Constructing wrinkles by utilizing strain-driven surface instability in film–substrate systems is a general method to prepare micronano structures, which have a wide range of applications in smart surfaces and devices such as flexible electronics, reversible wetting, friction, and optics. However, cracks generated during the preparation and use process significantly affect the uniformity of wrinkled surfaces and degrade the functional properties of the film devices. The realization of crack-free wrinkles with high stretchability in hard film systems is still a great challenge. Here, we report on a facile technique for controllable preparation of large-area, highly stretchable, crack-free wrinkled surfaces by ultraviolet ozone (UVO) treatment of Ecoflex. The thickness dependence of the wrinkles and the in situ wrinkling process during mechanical loading are investigated. The wrinkles including striped, labyrinth-like, herringbone, and transitional structures are controllable by changing strain mode (uniaxial or biaxial), loading history (simultaneous or sequential), strain anisotropy, and gradient loading. The wrinkled surfaces obtained using UVO-treated Ecoflex have tunable wetting and optical properties and can maintain excellent mechanical stability under large strains. This study provides a facile method for the preparation of large-area, crack-free wrinkles, which is simple, fast, low-cost, and robust. The resulting wrinkled surfaces remain stable under high stretching, which is beneficial for many practical applications, especially in the cases of large strains.