Borate bioactive glasses have gained attention in recent years due to their therapeutic and regenerative effects in vivo. However, borate bioactive glasses release alkaline ions, increasing the local pH and creating a toxic environment for cell culture studies. A partial compositional substitution of phosphate for borate can create a pH-neutral glass that does not significantly affect the local pH while still releasing therapeutic ions. In the present study, a series of Na-Ca-borophosphate bioactive glasses with different borate-to-phosphate ratios was evaluated in vitro and in vivo for cytotoxicity and angiogenic effects. Compared to more basic borate glasses, the pH-neutral glasses supported endothelial cell migration and stimulated greater blood vessel formation in a chick chorioallantoic membrane model. The results from this study indicate that these pH-neutral glasses are promising angiogenic biomaterials for use in tissue engineering and regenerative medicine.