In this study, thermoluminescence characteristics of un-doped and Dy-doped calcium tetraborate (CaB4O7) compounds are reported. The polycrystalline powder samples of un-doped and Dy-doped CaB4O7 were prepared by a solid-state reaction at high-temperature method. The identification and characteristics of the obtained compounds were determined by X-ray diffraction, Fourier transform infrared analysis, differential thermal analysis, thermogravimetric analysis, and scanning electron microscopy. The glow curves were obtained using a thermoluminescent reader. Neutron sensitivity, dose-response, and heating rate of CaB4O7 compounds were determined by using a bare Cf-252 mixed neutron + gamma (n + gamma) source, and dose response results are compared to those of Harshaw TLD-600 and TLD-700 neutron dosimeters ((LiF)-Li-6:Mg,Ti and (LiF)-Li-7:Mg,Ti). The sensitivity of CaB4O7:Dy (0.5%) sample is approximately 4.35 and 3.36 times higher than that of TLD-600 and TLD-700, respectively.