In this study the low-temperature sintering effects and improved piezoelectric properties of CuO-doped 0.69 Pb(Zr0.47Ti0.53)O3-0.31[Pb(Zn0.4Ni0.6)1/3Nb2/3]O3 ceramics were investigated. At high temperatures, a sintered Pb(Zr,Ti)O3–Pb(Zn,Ni)NbO3 material has excellent piezoelectric properties such as a high piezoelectric charge coefficient (d33), high electromechanical coupling coefficient (kp), and high relative dielectric permittivity (εr). However, low-temperature sintering of functional ceramics is important for industrial device applications. For sensor applications, sintering or fabrication temperature is important because processing temperatures can interfere with process and material compatibility. Therefore, in this study, low-temperature sintering effects were investigated by employing low-temperature sintering aids while maintaining the piezoelectric properties. CuO was selected as the sintering aid for these applications. We will investigate and discuss the effects of the low-temperature sintering aid of CuO on the Pb(Zr,Ti)O3–P(Zn,Ni)NbO3 material in device applications. By employing the CuO dopant to Pb(Zr,Ti)O3–P(Zn,Ni)NbO3 material, the strain and transduction values were increased while reducing the sintering temperature.