A sensitization procedure is used to enhance the thermoluminescence (TL) sensitivity of phyllite to emit radiation. Phyllite is a type of foliated metamorphic rock made from slate. This study examines naturally grown phyllite rock, which had not been previously studied. Using a Thermo 3500 manual reader, the TL sensitivity of phyllite as a function of dosage was measured. The doses required to perform this study were administered using a 60Co source. The statistical regression test of the data had a significance level of p < 0.05. The study also included thermal and pre-dose effects. Using the sensitization procedure, the nonlinearity in TL dose–response was removed, and the sensitivity was increased 44 times that of its original value. The fading study showed a dependence on the test dose. According to the obtained results, the combination of linear dose–response and high sensitivity to gamma radiation makes phyllite an important rock for dating and retrospective dosimetry.