In this paper, two different processing routes were adopted for the preparation of lead-free (Na0.52K0.44Li0.04)Nb0.87Sb0.08Ta0.05O3 ceramics and favorable results were obtained. The samples were characterized by X-ray techniques and scanning electron microscopy. Piezoelectric and dielectric data were presented. All the (Na0.52K0.44Li0.04)Nb0.87Sb0.08Ta0.05O3 samples possessed pure perovskite phase, and not any secondary phase could be certified. Excellent piezoelectric properties of d33=376pC/N, kp=44.1% and tanδ=2.4% were obtained for the composition compounded with (Na0.52K0.44Li0.04)NbO3 and (Na0.52K0.44Li0.04)Nb0.74Sb0.16Ta0.1O3 in the molar ratio 1:1. The remarkably strong piezoelectricity is probably due to the improved compositional homogeneity and enhanced densification achieved by the two-stage preparation method. The work will lead to further improvements in the properties of KNN-based piezoelectric materials.