In this study, powders of lead indium niobatelead titanate (1−x)Pb(In 1/2 Nb 1/2 )O 3 -(x)PbTiO 3 (PINT) binary system near the morphotropic phase boundary (MPB) composition with x=38 mol% PbTiO 3 are synthesized with the conventional mixed oxide and the wolframite methods via a rapid vibro-milling technique for the first time. The preparation method and calcination temperature have been found to show pronounced effects on the phase formation behavior of the PINT powders. The stabilized perovskite phase form of PINT can be synthesized by the wolframite method, while precursor phases are still found in powders prepared by the conventional method. Finally, this study shows that the rapid vibro-milling mixing technique is effective in preparing the phase pure perovskite of PINT powders.