This investigation has been performed to test the feasibility of using K2YF5:Tb3+ crystals as thermoluminescence dosemeters (TLD). K2YF5 single crystals doped with 0.2, 10.0 and 50.0 at.% of trivalent optically active Tb3+ ions as well as K2TbF5 and undoped K2YF5 crystals have been synthesized under hydrothermal conditions. Polished crystal platelets with thickness of about 1 mm have been irradiated with X and gamma rays in order to study thermoluminescent (TL) sensitivity as well as dose and energy response in terms of the Tb3+ concentration in K2YF5. Within this concentration series, K2YF5 crystals doped with 10.0 at.% Tb3+ have been found to have maximum TL response due to a broad asymmetric TL glow peak at 269 degrees C with good linearity of dose response and reproducibility of dose measurements. After deconvolution, the main dosimetric peak has been revealed to be composed of two individual peaks, both with linear TL response behaviour, centered at 210 and 269 degrees C. As it has been proved, the linear TL signal coefficient for K2Y0.9Tb0.1F5 is almost 10 times greater than that for commercial TLD-100 (LiF:Mg,Ti), irradiated with a 137Cs gamma radiation source at the same conditions. The reported results indicate that K2YF5 crystals doped with Tb3+ have potential as promising materials for radiation dosemeters.