The high mechanical quality factor (Q m ) of KNNbased ceramics is usually achieved by acceptor doping. However, this hardening effect has serious limitations due to the increased mobility of oxygen vacancies under large electric fields and hence is difficult to use in high-power applications. In this work, the hardening mechanism is demonstrated by the development composites of the 0.957(K 0.48 Na 0.52 )Nb 0.94 Ta 0.06 O 3 -0.04-(Bi 0.5 Na 0.5 )ZrO 3 -0.003BiFeO 3 (KNNT-BNZ-BFO) matrix with the K 4 CuNb 8 O 23 (KCN) phase using the two-step ball-milling method. A decrease in remnant polarization and dielectric constant and an increase in resistivity and Q m are observed compared to that in the KNNT-BNZ-BFO sample. A high Q m of 160, Curie temperature, T C , of 310 °C, and piezoelectric coefficient, d 33 , of 330 pC/N can be obtained simultaneously in the composite with a 0.008 mole ratio of KCN. This can be explained by the mechanical clamping effect of KCN due to strain incompatibility and the domain wall pegging that traps charges at the KNNT-BNZ-BFO/KCN interface. This composite approach is considered a general hardening concept and can be extended to other KNN-based ceramic systems.