Aerosol deposition method was used as an alternative deposition technique in crystalline electrolyte deposition process. Crystalline Li1.3Al0.3Ti1.7(PO4)3 thick layers were successfully deposited on stainless-steel substrates and X-ray diffractometry, scanning electron microscopy, transmission electron microscopy, and AC impedance techniques were used to characterize these films. The density of the deposited films was between 83% and 86% of the theoretical density and Vickers hardness was calculated to have values between 260 and 280 Hv. Bulk and total conductivities were 3.62 × 10−3 and 1.12 × 10−6 S/cm, respectively, and DC conductivity was <10−10 S/cm for a wide range of film thicknesses. Improvement in total conductivity of the Li1.3Al0.3Ti1.7(PO4)3 samples is still needed to make these films more suitable for all-solid-state Li-ion batteries.