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Electrospun nanofibers mimic the bone’s extra-cellular matrix and represent an alternative implant coating to enhance implant osseointegration. Approximately 99% of the strontium (Sr2+) in our body deposits in the bone and serves as a stimulator of bone formation. The purpose of this study was to develop an Sr2+-doped coaxial polycaprolactone (PCL)/poly(D,L-lactide-co-glycolide) (PLGA)-polyvinyl alcohol (PVA) nanofiber coating to enhance the osseointegration. An optimized PCL/PLGA (1:1 v/v) sheath fiber formula was identified to match the nanofibers degradation to the implant osseointegration physiology. Scanning electron microscopy images showed that the Sr2+-doped nanofibers had a less dense structure and larger porosity than the nanofibers without Sr2+ doping. A sustained Sr2+ release from the PCL/PLGA-PVA coaxial nanofibers was observed for over two months. The indirect and direct cellular contact studies confirmed the biocompatibility of the Sr2+-doped PCL/PLGA-PVA coaxial nanofibers. The Sr2+-doped nanofibers provided further and significant enhancement of the differentiation of murine pre-osteoblast MC3T3-E1 cells. These findings indicate that Sr2+-doped PCL/PLGA-PVA coaxial nanofibers have a great potential to be applied as a new implant coating matrices.