We introduce a comprehensive scheme to physically quantify both viscous and elastic rheological nonlinearities simultaneously, using an imposed large amplitude oscillatory shear (LAOS) strain. The new framework naturally lends a physical interpretation to commonly reported Fourier coefficients of the nonlinear stress response. Additionally, we address the ambiguities inherent in the standard definitions of viscoelastic moduli when extended into the nonlinear regime, and define new measures which reveal behavior that is obscured by conventional techniques.