In this study, the influence of the processing parameters, such as the synthesis temperature and the lithium sources on the structure, particle size, morphology and ionic conductivity of Li1+x Ti2−x Al x (PO4)3 (LTAPO) was investigated. LiNO3, LiCl, and Li acetate were employed as lithium sources for investigating the effects of Li sources on the properties of the solid electrolyte. The morphologies and the particle size distribution of the prepared LTAPO samples were analyzed by using scanning electron microscopy (SEM) and a laser particle size analyzer. Their crystallinities were measured by means of X-ray diffraction (XRD). An increase in the synthesis temperature caused a pronounced growth in the particle size without any impurities, especially at temperatures above 700 °C. In addition, LiCl lithium sources showed the highest particles size. The effect of the processing parameters on the ionic conductivity of the prepared LTAPO was investigated by using electrochemical impedance spectroscopy (EIS). The ionic conductivities of the LTAPO prepared by using an optimized synthesis temperature with different lithium sources were 8.36 × 10−4, 5.73 × 10−4, and 7.18 × 10−4 S/cm for C-LTAPO, A-LTAPO, and N-LTAPO, respectively. The properties of the ceramic solid electrolyte were shown to be affected by the choice of the synthesis temperature and the Li source material.