In the Hellenides Orogen, minerals of various gem quality occur in various rock types from mainly four tectono-metamorphic units, the Rhodope, Pelagonian, and the Attico-Cycladic massifs, and the Phyllites-Quartzites unit of Crete Island. In crystalline rocks, gemstones are related to both regional metamorphic-metasomatic processes (e.g., gem corundums, Mn-andalusite, thulite/clinothulite, spessartine, titanite, jadeite), and to the formation of late alpine-type fissures, such as, for example, quartz, albite, adularia and titanite. The Tertiary (and Mesozoic) magmatic-hydrothermal environments provide gem-quality sapphire, beryl, garnet, vesuvianite, epidote, fluorite, and SiO2 varieties. The supergene oxidation zone of the Lavrion deposit hosts gem-quality smithsonite and azurite. Coloration in the studied material is either due to various chromophore trace elements present in the crystal structure, or due to inclusions of other mineral phases. Future modern exploration methods combined with gemological investigations (such as treatment and faceting of selected stones), are necessary in order to obtain a better knowledge of the gemstone potential of Greece for its possible exploitation.