Methods to control and prevent polymer films from buckling are provided. Buckled morphologies are created by thermally cycling or mechanically compressing a substrate such as poly(dimethylsiloxane) (PDMS) coated with a polyelectrolyte multilayer film. By varying the dimensions of the surface topography relative to the buckling wavelength (e.g., pattern size is less than, equal to, and greater than the buckling wavelength) the orientation and the local morphology of the buckled films is controlled. Based on the information obtained, we demonstrate how to alleviate the unavoidable buckling by incorporating nanoparticles into the film. In addition, we studied the effect of the silica layer that results from oxygen plasma treatment and the critical temperature for permanent film buckling.