The invention provides "engineered" nonlinear nanocomposite materials with an extremely large ⁽³⁾ and fast temporal response along with optical properties that can be precisely tuned to satisfy the requirements of a particular application (e.g., optical, thermal, mechanical, etc.). In particular, the magnitude of the linear and nonlinear index of refraction can be adjusted substantially independently of the absorption spectrum of the material. In addition, the optical characteristics can be engineered substantially independently from the mechanical and chemical characteristics, providing exceptional performance and flexibility in terms of device-incorporation and process-stability.