Cardiovascular diseases (CVD) represent one of the most important causes of death all over the world. Consequently, many efforts are invested in their treatment and in the development of drugs that can be useful against these ailments. Plants and plant-derived drugs and functional foods are very important in this respect. On the one hand, molecules obtained from different species of the genus Digitalis (particularly D. lanata and D. purpurea), such as digitalin, digoxin and digoxigenin, are among the most relevant cardiotonic drugs and still come from their natural sources, since their synthesis would be complicated and expensive. On the other hand, many plants are used to cure, palliate or prevent heart, blood vessel and related illnesses at a popular level. As in many other fields of health, folk knowledge has led to both drug development in pharmaceutical industry and herbalist preparation production. Additionally, the direct plant management and use continues to be active at the popular level for this as well as for many other wellness-related purposes. Ethnobotanical research, which inventories the folk plant use in all domains, has been important since old times and has increased its focus on industrialised areas in the recent decades, where it continues to be practised currently. In this chapter we review the state-of-art of herbal medicines that are claimed to be useful for CVD in the Iberian Peninsula and the Balearic Islands. This territory (comprising three states, Andorra, Portugal and Spain, and a small area belonging to the United Kingdom) comprises one of the areas of highest plant biodiversity in Europe and an important linguistic and cultural diversity (Basque, Catalan, Galician, Portuguese, Spanish, and English in Gibraltar), this pointing to a very rich ethnobotanical knowledge. These territories being located in an industrial and economically developed area, certain ailments such as hypertension and hypercholesterolemia are frequent. In addition, functional foods play an important role in the Mediterranean diet, the one typical of the area, and, consequently, in the primary prevention of CVD. We record a total amount of 5,249 use reports of 784 taxa used against CVD. We analyse the existing ethnobotanical data linked to the cardiovascular system in the area considered, from our own results and from other relevant and representative sources. This review depicts a panorama of the folk use of herbal products to address the quoted ailments, and provides a basis for further (phytochemical, pharmacological and other) research, which could help in the development of medicinal products.