Bone regeneration strategies rely on biomaterial constructs with stem cells or growth factors. By comparison, cell homing strategies employ chemokines to recruit the host endogenous stem or progenitor cells to the defect site to support endogenous healing. In the present study, we used a novel fluffy hydroxyapatite/polyacrylonitrile (HA/PAN) composite scaffold to provide a better three-dimensional cell culture microenvironment. These HA/PAN composite scaffolds loaded with stromal cell-derived factor-1 alpha (SDF-1 alpha) provided a diffusion-controlled SDF-1 alpha release profile and endowed the scaffolds with cell homing capabilities. Furthermore, the scaffolds significantly stimulated bone marrow stromal cell (BMSC) recruitment, facilitated BMSC osteogenic differentiation, and promoted ectopic bone formation. Our results suggest that a HA/PAN composite scaffold loaded with SDF-1 alpha offers a clinically beneficial bone repair strategy.