The phosphate glass samples doped with Tb₂O₃ oxide (general formula: P₂O₅-Al₂O₃-Na₂O-Tb₂O₃) were synthesized and studied for usage in high-dose radiation dosimetry (for example, in high-activity nuclear waste disposals). The influence of terbium concentration on thermoluminescent (TL) signals was analyzed. TL properties of glasses were investigated using various experimental techniques such as direct measurements of TL response vs. radiation dose, T_max–T_stop and VHR (various heating rate) methods, and glow curve deconvolution analysis. The thermoluminescence dosimetry (TLD) technique was used as the main investigation tool to study detectors’ dose responses. It has been proved that increasing the concentration of terbium oxide in glass matrices significantly increases the thermoluminescence yield of examined material. For the highest dose range (up to 35 kGy), the dependence of the integrated thermoluminescent signals vs. dose can be considered as a saturation-type curve. Additional preheating of samples improves linearity of signal vs. dose dependencies and leads to a decrease of the signal loss over time. All obtained data suggest that investigated material can be used in high-dose radiation dosimetry. Additional advantages of the investigated dosimetric system are its potential ability to re-use the same dosimeters multiple times and the fact that reading dosimeters only requires usage of a basic TL reader without any modifications.