Atomic Force Microscopy (AFM) is a high-resolution analysis technique where an oscillating cantilever causes a very sharp tip (R ≈ 2-100nm) to interact with a sample surface and acquire mechanical property data. We apply established AFM techniques (e.g. Fast Force Volume, Tapping Mode, Force Modulation, etc), techniques developed within our research group and finite element analysis to measure and deconvolute the gradient of elastic and viscoelastic mechanical properties (known as the ‘interphase’) near the interfaces in polymer nanocomposites. The AFM is also a key tool for microstructure characterization as it can produce mechanical property contrast for samples, whereas other analysis techniques (e.g. scanning electron microscopy) are not able to differentiate between constituent components. To make AFM analysis suitable to inform material property predictions within the umbrella of the Material Genome Initiative, there is a continued focus on the development of ‘model samples’ which allows for a combinatorial approach to the collection of interphase data and produce statistically meaningful results for many different polymer-substrate configurations.