Lithium Triborate (LiB3O5 or LTB), is characterized by chemical stability and good mechanical properties, and it has an effective atomic number (Zeff = 7.39) close to that of the human tissue (Zeff = 7.42), making it a potential dosimeter. The objective of this research is to examine the Thermoluminescence (TL) features and dosimetric characteristics of both Cu-doped and Ag-doped LTB. The material was synthesized using the solid-state synthesis method and four different dopant levels were used for each element (0.1%, 0.5%, 1%, 3%); various techniques such as X-Ray Diffraction (XRD), Scanning Electron Microscopy (SEM) and Fourier Transform Infrared (FTIR) spectroscopy were used for structural and compositional characterization, for samples annealed at 500 °C for 1 h in all cases. Specific TL features were studied, such as TL glow curve shape, sensitization and sensitivity, fading behavior as well as kinetic characterization using two supplementary techniques, namely fractional glow technique and deconvolution analysis. The effect of each dopant element is different in the (same) lithium triborate matrix in terms of sensitivity. TL dosimetric peaks are yielded for both dopant elements; however, the optimum doping level is 3% for Ag but just 0.1% for Cu. Furthermore, the samples were irradiated at different doses, ranging from 0.5 to 2048 Gy, in order to study the corresponding dose response. A remarkable dose response linearity was observed for the main dosimetric peak of both materials, ranging up to ∼1 kGy.The fading results suggest that LTB doped with 0.1% Cu is the most promising material for dosimetric applications.