Nano-attapulgite (nano-ATP) has shown potential in promoting mesenchymal stem cell (MSC) adhesion, growth and osteogenic gene expression. In this study, we investigated a 3D-bioprinted porous Sr-ATP (strontium-doped nano-ATP)/GelMA/chitosan composite hydrogel scaffold for bone regeneration. The experiment was divided into four groups based on the concentration of Sr-ATP: control (0%), 0.5%, 1.0% and 2.0%. The primary novelty of our research lies in the incorporation of Sr-ATP, which enhances the biological and mechanical properties of scaffolds. Additionally, we utilized a stable Pickering emulsion templating technique combined with 3D printing to fabricate the scaffold, ensuring a uniform and stable porous structure. The biological and mechanical properties of the scaffold were evaluated in vitro, and its potential to promote angiogenesis and osteogenesis was assessed in vivo using cranial defect model. Our results indicate that the scaffold presents a promising solution for bone formation in bone defects, demonstrating significant improvements in both angiogenesis and osteogenesis.