Non-destructive, nanoscale characterization techniques are needed to understand both synthetic and biological materials. The atomic force microscope uses a force-sensing cantilever with a sharp tip to measure the topography and other properties of surfaces(1,2). As the tip is scanned over the surface it experiences attractive and repulsive forces that depend on the chemical and mechanical properties of the sample. Here we show that an atomic force microscope can obtain a range of surface and subsurface information by making use of the nonlinear nanomechanical coupling between the probe and the sample. This technique, which is called mode-synthesizing atomic force microscopy, relies on multi-harmonic forcing of the sample and the probe. A rich spectrum of first-and higher-order couplings is discovered, providing a multitude of new operational modes for force microscopy, and the capabilities of the technique are demonstrated by examining nanofabricated samples and plant cells(3,4).