Orbital bone damage (OBD) may result in severe post-traumatic enophthalmos, craniomaxillofacial deformities, vision loss, and intracranial infections. However, it is still a challenge to fabricate advanced biomaterials that can match the individual anatomical structure and enhance OBD repair in situ. Herein, we aimed to develop a selective surface modification strategy on bioceramic scaffolds and evaluated the effects of inorganic or organic functional coating on angiogenesis and osteogenesis, ectopically and orthotopically in OBD models. It was shown that the low thermal bioactive glass (BG) modification or layer-by-layer assembly of a biomimetic hydrogel (Biogel) could readily integrate into the pore wall of the bioceramic scaffolds. The BG and Biogel modification showed appreciable enhancement in the initial compressive strength (∼30−75%) or structural stability in vivo, respectively. BG modification could enhance by nearly 2-fold the vessel ingrowth, and the osteogenic capacity was also accelerated, accompanied with a mild scaffold biodegradation after 3 months. Meanwhile, the Biogel-modified scaffolds showed enhanced osteogenic differentiation and mineralization through calcium and phosphorus retention. The potential mechanism of the enhanced bone repair was elucidated via vascular and osteogenic cell responses in vitro, and the cell tests indicated that the Biogel and BG functional layers were both beneficial for in vitro osteoblastic differentiation and mineralization on bioceramics. Totally, these findings demonstrated that the bioactive ions or biomolecules could significantly improve the angiogenic and osteogenic capabilities of conventional bioceramics, and the integration of inorganic or organic functional coating in the pore wall is a highly flexible material toolbox that can be tailored directly to improve orbital bone defect repair.