Luminescent Y3Al5O12 : Eu3+ (YAG : Eu3+) and Y3Al5O12 : Tb3+ (YAG : Tb3+) powders with nanometre and micrometre-sized particles and films have been successfully synthesized by sol\textendashgel route from alkoxide precursors. Advanced YAG coatings were achieved by spray and dip-coating methods, giving rise to different structural and optical properties. High temperature x-ray diffraction, x-ray powder diffraction, scanning electron microscopy and atomic force microscopy were used to investigate the materials structure and morphology. Pure polycrystalline YAG powder was obtained from 900°C. Laser induced luminescence spectra as well as luminescence decays of Tb3+ and Eu3+ ions were recorded. This study showed, undoubtedly, the spectral features of an Eu3+ emitting centre embedded in a unique site of D2 symmetry. Furthermore, the well-known cross-relaxation phenomenon was observed for Tb3+. Decay times were found to be exponential and shorter than 5 ms for both Eu3+ and Tb3+ activators. Finally, the spectroscopic properties of YAG : Tb3+ powders under vacuum ultra violet excitation were analysed and encouraging results were obtained regarding luminescence efficiency and time constants.