The data presented has to do with identifying the various phases arising during the synthesis of the Y-type hexaferrite series Ba0.5Sr1.5Zn2-xNixFe12O22 by auto-combustion that we deem important for their microstructural and magnetic properties. The data and the related analyses support the research paper “Ni-substitution effect on the properties of Ba0.5Sr1.5Zn2-xNixFe12O22 powders” 1. Thus, the parameters are presented of the phases appearing after auto-combustion and after the initial annealing at 800 °C, namely, crystal cell and crystallite size. Also, additional data are provided obtained by EDS concerning the Ba:Sr:Zn:Ni:Fe ratio in Ba0.5Sr1.5Zn2-xNixFe12O22 (x = 0.8, 1, 1.5) samples synthesized at 1170 °C for 10 h. The data can be used as a reference in establishing how the phases distinguished during the initial process of auto-combustion affect the Ba0.5Sr1.5Zn2-xNixFe12O22 powders, which are candidates for room-temperature multiferroic materials. The data have not been published previously and are made available to permit critical or further analyses.