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The dielectric properties and synthesis of pyrochlore-free lead zinc niobate ceramics with Ba substituting for Pb were investigated. Ba partial substitution for Pb was effective in stabilizing the perovskite structure in PZN ceramics, where the minimum amount of Ba substitution needed was about 20 mol%. The dielectric loss and the temperature coefficient of dielectric constant of PZN were reduced markedly with Ba substitution, while the dielectric constant was greater than 110. Good dielectric properties were obtained for the composition of Pb0.3Ba0.7(Zn1/3Nb2/3)O3:ε = 133.5, tan δ = 0.0009, τε = −811 ppm/°C.