This work is focused on the synthesis of Aldoped yttrium-iron garnet ferrites via precipitation in aqueous solutions at controllably maintainedp H using different sequences for metal cations precipitation. The effect of different technological routes on the specifics of the crystalline structure formation and the temperature stability of the magnetic properties are studied in detail for Y3AlFe4O12 nanoparticles and bulk samples comprised of such nanoparticles. A comprehensive analysis of the results obtained yields the strategy for optimizing the synthesis roadmap for obtaining Al-doped yttrium-iron ferrite garnets with the desired set of physical properties for technological applications.