Graphene sheets functionalized covalently with biocompatible poly-l-lysine (PLL) were first synthesized in an alkaline solution. PLL-functionalized graphene is water-soluble and biocompatible, which makes it a novel material promising for biological applications. Graphene sheets played an important role as connectors to assemble these active amino groups of poly-l-lysine, which provided a very biocompatible environment for further functionalization, such as attaching bioactive molecules. As an example, an amplified biosensor toward H₂O₂ based on linking peroxidase onto PLL-functionalized graphene was investigated.