Highly sensitive sensor arrays are in high demand for prospective applications in remote sensing and imaging. Measuring microscopic deflections of compliant micromembranes and cantilevers is developing into one of the most versatile approaches for thermal, acoustic and chemical sensing. Here, we report on an innovative fabrication of compliant nanocomposite membranes with nanoscale thickness showing extraordinary sensitivity and dynamic range, which makes them candidates for a new generation of membrane-based sensor arrays. These nanomembranes with a thickness of 25-70 nm, which can be freely suspended over large (hundred micrometres) openings are fabricated with molecular precision by time-efficient, spin-assisted layer-by-layer assembly. They are designed as multilayered molecular composites made of a combination of polymeric monolayers and a metal nanoparticle intralayer. We demonstrate that these nanocomposite membranes possess unparalleled sensitivity and a unique autorecovering ability. The membrane nanostructure that is responsible for these outstanding properties combines multilayered polymer/nanoparticle organization, high polymer-chain orientation, and a pre-stretched state.