Graphite in the Borrowdale (Cumbria, UK) deposit occurs as large masses within mineralized pipe-like bodies, in late graphite–chlorite veins, and disseminated through the volcanic host rocks. This occurrence shows the greatest variety of crystalline graphite morphologies recognized to date from a single deposit. These morphologies described herein include flakes, cryptocrystalline and spherulitic aggregates, and dish-like forms. Colloform textures, displayed by many of the cryptocrystalline aggregates, are reported here for the first time from any graphite deposit worldwide. Textural relationships indicate that spherulitic aggregates and colloform graphite formed earlier than flaky crystals. This sequence of crystallization is in agreement with the precipitation of graphite from fluids with progressively decreasing supersaturation. The structural characterization carried out by means of Raman spectroscopy shows that, with the exception of colloform graphite around silicate grains and pyrite within the host rocks, all graphite morphologies display very high crystallinity. The microscale SIMS study reveals light stable carbon isotope ratios for graphite (δ ¹³C = −34.5 to −30.2‰), which are compatible with the assimilation of carbon-bearing metapelites in the Borrowdale Volcanic Group magmas. Within the main mineralized breccia pipe-like bodies, the isotopic signatures (with cryptocrystalline graphite being lighter than flaky graphite) are consistent with the composition and evolution of the mineralizing fluids inferred from fluid inclusion data which indicate a progressive loss of CO₂. Late graphite–chlorite veins contain isotopically heavier spherulitic graphite than flaky graphite. This agrees with CH₄-enriched fluids at this stage of the mineralizing event, resulting in the successive precipitation of isotopically heavier graphite morphologies. The isotopic variations of the different graphite morphologies can be attributed therefore, to changes in the speciation of carbon in the fluids coupled with concomitant changes in the XH₂O during precipitation of graphite and associated hydrous minerals (mainly epidote and chlorite).