Heart failure (HF) is a common and serious manifestation after myocardial infarction (MI). Despite their clinical importance, current treatments for MI still have several limitations. Revascularization has been proven to have positive effects on MI-induced damage. Currently biomaterial-based angiogenesis strategies represent potential candidates for MI treatment. Bioglass (BG) is a commercially available family of bioactive glasses. BG has angiogenic properties and thus might be an attractive alternative for MI treatments. Here, we loaded BG in sodium alginate (BG-SA), locally injected it into peri-infarct myocardial tissue and examined its suitability for inducing cardiac angiogenesis and eventually improving cardiac function following MI. Cardiac function was evaluated via echocardiography. Infarct morphometry, angiogenesis, apoptosis and angiogenic protein expression were all analysed 4 weeks after BG-SA injection. Compared with the control treatment, BG-SA was sufficient to prompt angiogenesis, suppress apoptosis, up-regulate the expression of angiogenic proteins, attenuate infarct size, preserve wall thickness and eventually improve cardiac function. Our results demonstrate the feasibility and effectiveness of BG-SA in myocardial regeneration via angiogenesis, suggesting that BG-SA is a potential therapeutic strategy for post-infarct myocardial regeneration.