Biomaterials have potential applications in the treatment of myocardial infarction (MI). These biomaterials have the ability to mechanically support the ventricular wall and to modulate the inflammatory, metabolic, and local electrophysiological microenvironment. In addition, they can play an equally important role in promoting angiogenesis, which is the primary prerequisite for the treatment of MI. A variety of biomaterials are known to exert pro-angiogenic effects, but the pro-angiogenic mechanisms and functions of different biomaterials are complex and diverse, and have not yet been systematically described. This review will focus on the pro-angiogenesis of biomaterials and systematically describe the mechanisms and functions of different biomaterials in promoting angiogenesis in MI.