A series of compositions in the Pb(Zn 1/3 Ta 2/3 )O 3 –Pb(Fe 1/2 Nb 1/2 )O 3 system were prepared and characterized. Ceramic powders were synthesized via a two-step B-site precursor route. Perovskite formation yields increased with the Pb(Fe 1/2 Nb 1/2 )O 3 fraction. Weak-field low-frequency dielectric properties of the densified ceramics were investigated, where diffuse modes in the phase transition were observed at several compositions. Fractured samples were explored for the examination of the internal microstructure.