In this paper, a novel strategy to control the orientation of nanowrinkles by applying a thickness-gradient to a bilayer-system is presented. Surface modification by plasma treatment on ultraviolet light-curable polysiloxane-based resin applies biaxial compressive strain, resulting in the formation of randomly oriented nanowrinkles over a large-area. The thickness-gradient of the resin, given by the meniscus formed between the groove made with patterned polydimethylsiloxane (PDMS) after spin-coating of the resin, directed wrinkle propagation. Given the propagation orientation, nanowrinkles were well aligned over a large-area using a simple and accessible method.