Calcium phosphate (CaP) bioceramics are broadly employed for bone regeneration due to their excellent biocompatibility and osteoconductivity. However, they are not capable of repairing healing-impaired bone defects such as defects with conditions of ischemia or infection due to restricted bioactivities. In this study, we synthesized single-phased strontium-zinc-phosphate (SZP, SrZn2(PO4)2) bioceramics via a solution combustion method and further fabricated SZP scaffolds using a three-dimensional (3D) printing technique. Compared to 3D printed β-tricalcium phosphate (β-TCP) scaffolds, the 3D printed SZP scaffolds presented comparable porosity, compressive strength, and Young's modulus, but increased ability of osteogenesis, angiogenesis, immunomodulation and anti-bacterial activity. Specifically, 3D printed SZP scaffolds not only led to significantly higher osteogenic differentiation of MC3T3-E1 cells and pro-angiogenesis of human umbilical vein endothelial cells (HUVECs) directly or through macrophage-mediated immunomodulation, but also inhibited the growth of Staphylococcus aureus (S. aureus) and Escherichia coli (E. coli). The in vivo study of the rat cranial bone defect model further confirmed better vascularized bone regeneration in 3D-printed SZP scaffolds. These findings indicate that the proposed 3D-printed SZP scaffolds might be a versatile candidate for bone tissue engineering.