Surface modification of titanium is encouraged to facilitate early osseointegration in dental and orthopedic fields. Icariin is the main active constituents of Herba Epimedii, which has good bone-promoting ability. We established an icariin-functionalized coating composed of icariin and poly (lactic-co-glycolic acid) (PLGA) on TiO2 nanotubes surface (NT-ICA-PLGA) to promote osteoblast cell activity and early osseointegration. Surface topography, wettability and drug release pattern of the established NT-ICA-PLGA surface were characterized by scanning electron microscopy (SEM), contact angle test and drug release test. MC3T3-E1 osteoblast cell activity tests were performed using SEM, immunofluorescent staining, cell counting kit-8 and alkaline phosphatase assays. The osteogenic effects of different surfaces were observed using a rat model. Surface characterization proved the successful fabrication of the icariin-functionalized coating on the TiO2 nanotube structure, with increased wettability. The NT-ICA-PLGA substrate showed sustained release of icariin until two weeks. Osteoblast cells grown on the NT-ICA-PLGA substrate displayed improved cell adhesion, proliferation and differentiation ability than the control Ti surface. The in vivo experiment also revealed superior bone forming ability on the NT-ICA-PLGA surface, compared to the pure Ti control. These results imply that the developed NT-ICA-PLGA substrate has a promising future use as functionalized coating for implant surface modification.