Zinc Magnesium Aluminate doped with Dysprosium (Zn (1-x-y) Mg(y)Al2O4:x Dy (x=0.04 and y=0.3 mol%)) was prepared using the solution combustion synthesis method. The prepared phosphor was characterized using energy-dispersive X-ray spectroscopy, scanning electron microscopy, X-ray diffraction, transmission electron microscopy, and Fourier transform infrared, respectively, to study crystal structure, surface morphology, and vibrational properties. The thermoluminescence peak temperatures were 250°C, 248°C, and 246°C at irradiating doses of 600–1000 Gy, respectively. Through the computation of the activation energy (E), order of kinetics (b), and frequency factor (s−1), the kinetic parameters were assessed using the TL glow curve. It is observed from the TL dose-response curve that the intensity rises nearly linearly for all doses between 600 and 1000 Gy. Nanophosphor Zn0.66Mg0.3Al2O4:0.04Dy shows almost linear dose-response for a dose range of 600–1000 Gy and an optimum activation energy (E) of 0.93–0.97 eV, which makes it suitable for high-dose radiation thermoluminescence dosimetric applications.