MnO2-doped 0.985[Li0.04(Na0.545K0.46)0.96(Nb0.81Ta0.15Sb0.04)]O3+0.015KNbO3(0.985LNKNTS+0.015KNbO3)lead-free ceramics were fabricated by conventional solid state method to develop excellent dielectric andpiezoelectric properties. The result of X-ray diffraction patterns obviously indicated that all of thespecimen has pure perovskite structure without secondary phase. In addition, orthorhombic phase andcoexistance region of orthorhombic-tetragonal phase (MPB) were observed with amount of MnO2. Theoptimal values of ρ=4.70 g/cm3, d33=238 pC/N, kP=0.46, Qm=121, εr=849, and TC=225℃ were obtained at0.01 mol% MnO2 doped 0.985LNKNTS+0.015KNbO3 ceramics sintered at 990℃ for 5 h, respectively. Hence, it was indicated that the suitable amount of MnO2 could improve the electrical properties of0.985[Li0.04(Na0.545K0.46)0.96](Nb0.81Ta0.15Sb0.04)]O3+0.015KNbO3 ceramics.