Li2O excess 0.95(Na0.5K0.5)NbO3-0.05LiTaO3 (NKN-5LT) ceramics were developed by conventional sintering method. Abnormal grain growth in NKN-5LT ceramics was observed with varying Li2O content during sintering. In the 1 mol% Li2O excess NKN-5LT samples sintered at 1000 oC for 4h in air, electromechanical coupling factor and piezoelectric constant of NKN-5LT ceramics were found to reach the highest values of 0.37 and 250 pC/N, respectively. Lead-free piezoelectric of the composition 1 mol% Li2O excess NKN-5LT were fabricated. 10×10×3 mm3 size multilayer ceramic actuators (MLCA) were fabricated by conventional tape casting method. The displacement of the MLCA was ~ 1 μm at 150 V. These results show that the NKN-5LT ceramics with reasonable good piezoelectric properties have the potential to become the next generation material for a wide range of electro-mechanical transducer applications.