A method of creating crumples in a monolayer entails contacting a monolayer comprising a two-dimensional material with a thermally contractible polymer, and heating the thermally contractible polymer to contract the polymer and induce buckling of the monolayer, where a plurality of crumples are formed in the monolayer due to the buckling. A device having a crumpled microstructure includes a monolayer comprising a two-dimensional material and including a plurality of crumples.