n this paper, in order to develop outstanding Pb-free composition ceramics, the Fe2O3-doped(Na0.525K0.443Li0.037)(Nb0.883Sb0.08 Ta0.037)O3 + 0.3 wt% Bi2O3 + x wt% Fe2O3 (x= 0∼1.0 wt%)(abbreviated as NKL-NST) lead-free piezoelectric ceramics have been synthesized using the ordinary solid state reaction method. The effect of Fe2O3-doping on their microstructure and electrical properties were investigated. XRD diffraction pattern studies confirm that Fe2O3 completely diffused into the NKL-NSTlattice to form a new stable soild solution with Fe3+ entering the Nb5+, Sb5+ and Ta5+ of B-site. And, phase structure of all the ceramics exhibited pure perovskite phase and no secondary phase was found in the ceramics. The ceramics doped with 0.6 wt% Fe2O3 have the optimum values of piezoelectric constant(d33), planar piezoelectric coupling coefficient(kp) and mechanical quality factor(Qm) : d33= 233[pC/N], kp= 0.44, Qm= 95. These results indicate that the (Na0.525K0.443Li0.037)(Nb0.883Sb0.08Ta0.037)O3 +0.3 wt%Bi2O3 + 0.6 wt% Fe2O3 ceramic is a promising candidate for lead-free piezoelectric ceramics.