Cardiovascular disease (CVD) is one of the most critical diseases which is the predominant cause of death in the world. Early screening and diagnosis of the disease and effective treatment after diagnosis play an important role in the patient's recovery. Metal-organic frameworks (MOFs), a kind of hybrid ordered micro or meso-porous materials, constructed by metal nodes or clusters with organic ligands, due to their special features like high porosity and specific surface area, open metal sites, or ligand tunability, are widely used in various areas including gas storage, catalysis, sensors, biomedicine. Recently, advances in MOFs are bringing new developments and opportunities for the healthcare industry including the theranostic of CVD. In this review, the applications of MOFs are illustrated in the diagnosis and therapy of CVD, including biomarker detection, imaging, drug delivery systems, therapeutic gas delivery platforms, and nanomedicine. Also, the toxicity and biocompatibility of MOFs are discussed. By providing a comprehensive summary of the role played by MOFs in the diagnosis and treatment of CVDs, it is hoped to promote the future applications of MOFs in disease theranostics, especially in CVDs.