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The garnet-type solid Li-ion conductor, Li6.4La3Zr1.4Ta0.6O12, is viewed as a promising solid-state electrolyte for the next-generation high-performance Li-ion battery because of its high ionic conductivity and stability. The previous researches, in order to avoid Li volatilization loss during solid-state reaction of sintering, mother powder with the same composition as green bodies was usually used to cover the samples, it would waste the expensive raw materials and increase the fabrication cost. In this study, a new method was proposed to prepare the Li6.4La3Zr1.4Ta0.6O12 ceramic solid-state electrolyte where the Li loss is compensated by the outside Li2CO3. Samples prepared by this method have pure garnet phase and compact micromorphology with few pores. These samples have a high Li-ion conductivity of 2.9×10−4 S/cm and a low activation energy of 0.37 eV at room temperature. The electronic conductivity is 1.08×10−8 S/cm, which can be neglected for solid-state electrolyte. [ABSTRACT FROM AUTHOR]