Picosecond time resolved photoluminescence and photoconductivity measurements are performed to investigate the influence of high intensity illumination on the properties of Fullerene crystals. A highly nonlinear dependence of both the photoluminescence characteristics and the photoconductive response of the fullerenes is seen and temperature dependent measurements indicate that the nonlinear processes are associated with an insulatormetal-like phase transition in the material, and thus that the electronic properties of the excited state are dramatically altered at high excited state densities. The observed behaviour is compared and contrasted to the changes in the optical properties upon photochemical modification of the pristine material via Raman spectroscopy. Application of a simple phenomenological model to calculate the contribution of intermolecular exchange and correlation energies in the excited state supports the proposal that the observed phenomena originate from a Mott-like phase transition. A further manifestation of this behaviour is the emergence of a broadband electroluminescent emission above a critical injection current density.