Although angiopoietin-1has potential therapeutic use in angiogenesis, the biological role of angiopoietin-4, especially in its immobilized form, is already unknown. In this study, vascularization potential of angiopoietin-4 either alone or in combination with vascular endothelial growth factor (VEGF) was investigated following its immobilization onto the poly(2-hydroxyethyl methacrylate)-based bone scaffolds. Poly(2-hydroxyethyl methacrylate) (pHEMA)-based superporous hydrogels (SPHs) were synthesized by radical polymerization of hydroxyethyl methacrylate in the presence of gelatin or chitosan and the porosity was achieved by gas foaming. However, only pHEMA-gelatin SPHs fulfill the structural and biological characteristics of a bone scaffold. Therefore, angiopoietin-4 and/or VEGF were immobilized successfully onto the pHEMA-gelatin SPHs using carbodiimide chemistry. The cell culture studies that were performed with human umbilical vein endothelial cells (HUVECs) for 28days showed that immobilized angiopoietin-4 supported sprout formation more than that of other groups, while the immobilized VEGF including scaffolds promoted proliferation of HUVECs.