- Typical feature of high-fired medieval gypsum mortars is a compact microstructure of squat gypsum crystals containing firing products as remains of the calcination process. So far, the burning history of the binder is estimated based on morphological characteristics of the latter. A novel Raman microspectroscopy approach provides access to the calcination temperatures of individual anhydrite grains based on quantifiable spectroscopic changes appearing due to gradual variations of crystallinity, as independently confirmed by X-ray diffraction analysis of anhydrites synthesised at temperatures between 500°C and 900°C. The approach was successfully applied to the high-fired gypsum mortar of a South Tyrolean stucco sculpture of a pieta dated around 1420. Microparticles of burned anhydrite II with firing temperatures scattered around 650°C and clusters of thermally damaged natural anhydrite II crystals from the raw material were identified and imaged.