The significance of syngenetic and epigenetic graphite occurrences from the Variscan high-temperature/low-pressure Aracena Metamorphic Belt is discussed in the framework of the tectono-thermal evolution of this southern zone of the Iberian Massif. Syngenetic graphite is associated with both low- to medium-grade metamorphic rocks (La Umbría series, Precambrian in age) and high-grade, granulite facies rocks (the Precambrian Fuente del Oro series and a Cambrian calc-silicate series). Epigenetic, fluid-deposited occurrences correspond to overgrowths on existing metamorphic graphite grains and vein-type mineralization. Two types of graphitized particles with remarkable differences in reflectance, anisotropy and size can be distinguished in the Precambrian metapelites of the La Umbría series. Large, >150 μm length, platy crystals with high reflectance and anisotropy are interpreted as detrital and are considered indirect evidence of an old orogenic cycle prior to the Cadomian Orogeny, during which metamorphism exceeded greenschist facies. The coexistence of two types of particles explains the scattering of values of the c parameter of graphite determined by XRD (c = 6.72–6.74 Å), and the anomalously high temperatures of the DTA exothermic peak (close to 600 °C) of graphite with respect to that inferred from mineral assemblages in these rocks. The presence of graphite-rich quartzites and gneisses within the Fuente del Oro series and the calc-silicate series is evidence of sedimentation under reducing conditions in a continental shelf. The characteristics of graphite reflect the high-grade metamorphic conditions attained in the southern area of the Aracena Metamorphic Belt. Pervasive flow of fluids related to a major Variscan extensional event resulted in overgrowths on the pre-existing graphite in the gneisses and quartzites of the calc-silicate series, as evidenced by the heterogeneous isotopic composition of graphite single crystals in these rocks. A later stage of graphite precipitation is represented by scarce vein-type occurrences in mafic granulites that document channelled flow of fluids.