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CaZrO3-modified (K0.48Na0.48Li0.04)(Nb0.95Sb0.05)O3 (CZ-KNLNS) lead-free piezoelectric powders were synthesized by microwave method followed by conventional solid state sintering. Different amounts of CaZrO3 were added (i.e. x = 0, 0.02, 0.03, 0.04, 0.06 mol) and their effects on the crystal structure, microstructure, as well as the electrical properties, were investigated. The results showed that CZ-KNLNS powders could be obtained by microwave heating at a relatively low temperature and short time of 650 °C and 10 min, respectively. The obtained CZ-KNLNS powders have cubic structure and good crystallinity with average particle size of 300–700 nm. The particle size gradually decreases with the increase of CaZrO3 amount, indicating that addition of CaZrO3 inhibits the growth of the particles. The powders were further sintered at 1120 °C for 4 h and CZ-KNLNS ceramics with homogeneous and highly dense microstructure were obtained. X-ray diffraction showed that, with increasing CaZrO3 content, the phase structure gradually changed from orthorhombic to rhombohedral, which can be considered as the coexistence zone of orthorhombic-rhombohedral (O-R) phase in the range of 0.03 < x < 0.06. The optimized content of CaZrO3 is x = 0.04, at which the CZ-KNLNS piezoelectric ceramics show good properties and maximum d33 = 201.2 pC/N and Kp = 36.8%.