At the northwestern margin of the Gurktal Alps (Eastern Alps), Eoalpine (Cretaceous) thrusting of carbonaceous material (CM) bearing metasediments formed a very low- to low-grade metamorphic nappe stack above higher-grade metamorphic basement nappes. Sedimentary burial as well as progressive metamorphism transformed the enclosed CM to anthracite, metaanthracite and semigraphite. In a kinematically well-constrained section at the northwestern frontal margin of the nappe stack, this transformation has been investigated by vitrinite reflectance measurements and Raman spectroscopy of carbonaceous materials (RSCM). Automated, interactive fitting of Raman spectra estimates the metamorphic peak temperatures in a complete section through the upper part of the Upper Austroalpine unit. A RSCM trend indicates a temperature profile of ca. 250–600 °C. The top part of the gradient is reconstructed by one-dimensional thermal modeling. The certainty of ca. ± 25 °C at a confidence level of 0.9 resembles the data variability within a sample location. Due to the large calibration range, the method is able to reconstruct a thermal crustal profile in space and time. The study highlights the versatility of RSCM, which characterizes almost 250 Ma of a complex and polyphase tectonic history. RSCM data characterize the Variscan metamorphic grade in nappes now imbricated in the Eoalpine nappe stack. They additionally constrain a numerical model which emphasizes the significance of an increased thermal gradient in a continental margin towards the western Neotethyan ocean during Permo-Triassic lithospheric extension. It finally characterizes the Eoalpine metamorphic gradient during nappe stacking and a significant metamorphic jump related to exhumation and normal faulting.