The quest to identify low-cost thermoluminescence (TL) materials is vital, and the identification and assessment of natural materials suitable for radiation detection is a rapidly growing area of research. In addition to their specific dosimetric characteristics, such materials must be rigid, insoluble, and chemically inert. One such promising low-cost material can be a limestone having vast deposits in Pakistan. The present study reports the TL and dosimetric features of Pakistani limestone pellets and their comparison with TLD-100.The quarried crystalline limestone rock was hand crushed, sieved, and compressed into the standard TLD chip-sized pellets. The TL response, kinetic parameters, batch homogeneity, dose linearity, individual sensitivity correction factor (i.e., elemental correction coefficient ECC), lowest detectable dose limit (LDDL), coefficient of variation (COV), energy dependency, and fading were determined, and compared with TLD-100. For TL analysis, the pellets were exposed to an 8 Gy dose of 250 kVp X-rays. These exhibited complex TL showing four peaks (P1: 90–110 °C, P2: 130–170 °C, P3: 240–280 °C and P4: 320–350 °C). The limestone response was linear in the studied dose range of X-rays (1–10 Gy), unlike the supra-linear behavior of TLD-100. The kinetic parameters (i.e., the frequency factor (f), activation energy (E), and the kinetic order (b)) were estimated through computerized glow curve deconvolution using the general order of kinetics while confirmed by the Tm-Tstop method. The values of E and f were observed in the ranges of 0.85–1.27 eV and 5.98 × 107 to 1.81 × 1013 s−1, respectively. The calculated value of figure-of-merit (FOM) (i.e., 2.37%) showed a good agreement between the experimental and fitted glow curves. The overall variation in the ECCs for TLD-100 and limestone was found within ±4% and ±7%, respectively. The results of the ECC confirmed batch homogeneity. The calculated value of LDDL was ∼1.01 Gy. The investigation found that the maximum variation in normalized intensity and COV was within the tolerance limit of 5%. The limestone pellets showed less sensitivity than TLD-100. Like TLD-100 at high energy, the pellets showed an independent response. In contrast to TLD-100, the limestone pellets showed a higher response dependency for low-energy X-rays.During the fading study, the total TL intensity decreased by 20% within the initial 24 h of irradiation and then sustained stability for the subsequent week. The results of this study indicate that limestone pellets are effective as an X-ray dosimeter for doses between 1 and 10 Gy.