Mechanical properties and biological inertness of titanium provide potential in orthopedic and dental implants. However, integration of titanium-based implants into the existing tissue is a major problem. Herein, we demonstrate biofunctionalization of titanium surfaces through a mussel-inspired adhesion mechanism conjugated to self-assembled peptide nanofibers in order to overcome biocompatibility issues. A Dopa conjugated peptide nanofiber coating was used along with bioactive peptide sequences for osteogenic activity to enhance osseointegration of medical grade titanium surface, TiAl6V4 alloy. Dopa-mediated immobilization of osteogenic peptide nanofibers on titanium surfaces created an osteoconductive interface between osteoblast-like cells and inhibited adhesion and viability of soft tissue forming fibroblasts compared to the uncoated titanium substrate. This biofunctionalization strategy can be extended into other surface immobilization systems owing to the versatile adhesive properties of Dopa and the ease of ligand conjugation to peptide amphiphile molecules. © 2012 The Royal Society of Chemistry.