We demonstrate a high yield method of functionalizing graphene nanosheets through nitrene addition of azido-phenylalanine [Phe(N₃)] to exfoliated micro-crystalline graphite (μG). This method provides a direct route to highly functionalized graphene sheets. TEM analysis of the product shows few layer (n < 5) graphene sheets. The product was determined to have 1 phenylalanine substituent per 13 carbons.