Hybrid microelectromechanical systems (MEMS) based on microcantilevers (MCs) that exhibit very large chemi-mechanical responses are described. The principle method for enhancing response involves introducing metallic nanostructure to one side of the MC. This serves to increase surface area and create new modes of analyte-induced surface stress. Methods of fabricating these cantilevers are described. Bending of these MCs upon exposure to both gas phase and liquid phase analytes have been shown to be as much as two orders of magnitude greater than for conventional smooth surface cantilevers. The utility of these systems for sensing and actuation are discussed and demonstrated. The nanostructured cantilevers also exhibit potential as substrates for surface enhanced Raman scattering (SERS). The capability of these devices to function as hybrid MEMS, combining large mechanical responses to analytes with an ability to obtain distinctive SERS spectra, will be shown.