To be better used as medical implants in orthopedic and dental clinical applications, titanium and titanium-based alloys need to be capable of inducing osteogenesis. Here we describe a method that allows the facile decoration of titanium surfaces to impart an osteogenesis capacity. A Ti surface was first deposited on a poly(OEGMA-r-HEMA) film using surface-initiated atom-transfer radical polymerization (SI-ATRP) with the further step of carboxylation. The modified surfaces were resistant to cell adhesion. Fibronectin (FN) and recombinant human bone morphogenetic protein-2 (rhBMP-2) were further immobilized onto p(OEGMA-r-HEMA) matrices. Our results demonstrate that the FN- and rhBMP-2-conjugated polymer surfaces could induce the adhesion of MC3T3 cells on Ti surfaces. Moreover, the protein-tethered surface exhibited enhanced cell differentiation in terms of alkaline phosphatase activity compared to that of the pristine Ti surface at similar cell proliferation rates. This research establishes a simple modification method of Ti surfaces via Ti-thiolate self-assembled monolayers (SAMs) and SI-ATRP and identifies a dual-functional Ti surface that combines antifouling and osseointegration promotion.