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A suite of slate samples collected along a 2 km transect crossing the Lishan fault in central Taiwan were evaluated to assess the role of ductile deformation in natural graphitization at lower greenschist facies metamorphic conditions. The process of natural aromatization, or graphitization, of an organic precursor is well established as a thermally driven process; however, experimental studies have shown that the energy provided by deformation can substantially reduce the activation energy required for graphitization. This study provides a natural example of deformation‐induced graphitization. A strain gradient approaching the Lishan fault was established by scanning electron microscope imaging and X‐ray diffraction analysis of phyllosilicates and quartz that showed an increase in the strength of slaty cleavage development via dissolution‐precipitation processes. Thermal conditions were constrained to be near isothermal using calcite‐dolomite geothermometry. Raman spectroscopic results from carbonaceous material, including D1‐full width‐at‐half‐maximum (FWHM), G‐FWHM, Raman band separation (RBS), and a lesser‐known vibrational mode B2g‐FWHM, showed robust linear trends across the same sampling transect. However, the G‐FWHM parameter showed a trend opposite of that expected from thermally driven graphitization. The Raman results are interpreted to reflect a strain‐driven reduction in graphite crystallite size (decrease in G‐FWHM) but improvement in structural ordering in individual coherent domains. A multiple linear regression with an R2 value of 0.92 predicts the graphite D1‐FWHM values from the XRD‐derived ratio of muscovite populations and muscovite microstrain, demonstrating the concomitant recrystallization of silicates and carbonaceous material across the strain gradient, despite the disparate processes accommodating the deformation. This study demonstrates the role of deformation in natural graphitization and provides a new perspective on the use of graphite as a geothermometer in strongly deformed greenschist facies rocks. [ABSTRACT FROM AUTHOR]