To investigate the influence of K/Na ratio on the phase structure and electrical properties, 0.96 (K x Na 1−x ) NbO 3 -0.04 (Bi 0.5 Na 0.5 ) ZrO 3 lead-free piezoceramics with x=0.35~0.60 were prepared by a conventional solid-state reaction method. The results indicate that a typical phase boundary of orthorhombic-tetragonal (O-T) exists at x=0.39-0.55 by refining the K/Na ratio. The grain size of the ceramics becomes much larger as the K/Na increases, and the chemical compositions well keep in the ceramic matrix. The ceramics with x=0.39 show enhanced electrical properties (e.g., d 33 =275 pC/N, k p =34.5 %, T C =330°C,P r =27.5 μC/cm 2 , and E C =10.5 kV/cm). It is considered that the observed enhanced piezoelectricity should be ascribed to the phase coexistence of O and T phases of the ceramics.