The Zn/Li codoped 0.83Pb(Zr1/2Ti1/2)O3-0.11Pb(Zn1/3Nb2/3)O3-0.06Pb(Ni1/3Nb2/3)O3(PZT-PZN-PNN) piezoelectric ceramics were prepared by the conventional solid state method. The influences of different content of Zn/Li addition on the phase structure, the microstructure, and electrical properties were investigated. The results showed that the phase structure was shifted from the rhombohedra to tetragonal with the increase of Zn/Li content. The dielectric constant εr, the piezoelectric coefficient d33, and the electromechanical coupling coefficient kp increased firstly and then decreased, while the dielectric loss tanδ and mechanical quality factor Qm showed the opposite trend. The optimal piezoelectric properties with d33 of 513 pC/N，kp of 0.635， εr of 1 694，and tanδ of 0.023 5 were obtained when the Zn/Li content was 1wt%. The ceramics are expected to be used in the fabrication of low temperature co-fired laminated piezoelectric devices.