The present article is the first comprehensive review on the chemical composition and pharmacological activities of the raw materials of Crocus species. In the present review, data on chemical constituents and pharmacological profile of Crocus sativus stigmas, as well as of other plant parts (perianth, stamens, leaves, corms) of different Crocus spp. are given. This review discusses all the classes of compounds (carotenoids, flavonoids, anthocyanins, terpenoids, phenol carboxylic acids, etc.) detected in raw materials of Crocus plants providing information on the current state of knowledge on phytochemicals of Crocus species. Almost all structural formulas of the compounds identified and isolated from Crocus species are given; all compounds are presented in accordance with the types of the studied raw materials. The latest hypotheses relating to the biosynthesis pathways of the main biologically active compounds of saffron (crocin, picrocrocin, safranal), as well as chemotaxonomy of Crocus genus are briefly summarized. The present review discusses the most thoroughly studied pharmacological activities (namely, antioxidant, antiparasitic, hypolipidemic, antihypertensive, immunomodulatory, antimicrobial, antitumor, cytotoxic, antidepressant) of saffron stigmas extracts, of its individual phytochemicals (safranal, crocin, crocetin), as well as pharmacological activities of raw materials of other Crocus species. This comprehensive review will be informative for scientists searching for new properties of saffron stigmas, as well as for saffron producers, since the present review highlights the prospects for the use of waste products in the production of the expensive spice. In addition, the present review provides information on pharmacological properties and composition of other Crocus species as promising medicinal and food plants. In the present review the emphasis will be put on the chemical constituents of Crocus species and the intraspecies variation in phytochemicals and pharmacological activities.