Flexible, bendable, stretchable devices represent the future of electronics for a wide range of real-world applications. Due to the fact that these technologies deviate significantly from traditional wafer technologies there is a need to understand and engineer material systems that allow large elastic deformations present in such devices, which requires knowledge about the mechanical properties of these material systems. Here we evaluate the mechanical properties of a bilayer polydimethylsiloxane (PDMS)/silicon nanocrystal system. By observing the formation of instabilities due to finite bending deformation and applying theoretical modeling, we estimated the neo-Hookean coefficient (analogous to shear modulus at low stress/strain) of the silicon nanocrystal film to be 345 ± 23 kPa. The method used here represents a novel approach to evaluating these properties and is widely applicable to many different combinations of systems of nanocrystals and elastomers.