Lead-free piezoelectric 0.06(LiNbO3)–0.94(Na0.5K0.5)NbO3 (LNKN) ceramics in disc form were fabricated and characterized to acquire good electromechanical properties. A molding method including cold isostatic pressing (CIP) was used to form a dense and regular microstructure and suppress the cracking problems of LNKN ceramics during the following high-temperature sintering. The LNKN ceramic sintered at 1040 °C showed a high piezoelectric constant d
33 of 170 pC/N owing to its high density. Furthermore, perovskite LNKN films with the same composition as the ceramics were fabricated using 2-methoxyethanol-based sol–gel solution. The sol–gel surface coating on the LNKN ceramics was found to be very effective for increasing the piezoelectric constant because of the interface stabilization effect leading to a uniform electric field in piezoelectric elements. As a result, we obtained the highest piezoelectric constant d
33 of 183 pC/N. The lead-free LNKN ceramics are promising for applications in eco-friendly ferroelectric and piezoelectric devices.
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