We report a single-step strategy to achieve heterogeneous, three-dimensional (3D) texturing of graphene and graphite by using a thermally activated shape-memory polymer substrate. Uniform arrays of graphene crumples can be created on the centimeter scale by controlling simple thermal processing parameters without compromising the electrical properties of graphene. In addition, we show the capability to selectively pattern crumples from otherwise flat graphene and graphene/graphite in a localized manner, which has not been previously achievable using other methods. Finally, we demonstrate 3D crumpled graphene field-effect transistor arrays in a solution-gated configuration. The presented approach has the capability to conform onto arbitrary 3D surfaces, a necessary prerequisite for adaptive electronics, and will enable facile large-scale topography engineering of not only graphene but also other thin-film and 2D materials in the future.