These datasets include Raman spectral parameters collected from a) tube furnace-pyrolysed charcoals, made from Calluna vulgaris (Ling Heather) at 400, 600, 800 and 1000 degrees centigrade, and b) wildfire charcoals (Calluna vulgaris) produced and collected during a prescribed heathland burn in Aberdeenshire, Scotland. Accompanying these data includes thermocouple (fire temperature) readings from the heathland fire, corresponding directly to charcoal samples analysed using Raman spectroscopy (b). With regards to the derivation of this Raman data, deconvolution utilising two first order bands (D & G) was implemented, and median values for each spectrum were produced. Following this, D- and G-band width (FWHM), intensity (ID/IG or 'R1') and area (AD/AG) ratios, band separation (G-D or 'RBS'), and band width ratio (FWHMRa) parameters were calculated and applied. For geothermometry of wildfire charcoals, a linear equation was determined from FWHMRa median values - produced by the spectroscopy of tube furnace charcoals between 400 and 1000 degrees centigrade (a).