Ceramics with formula (1-x-y)[Na0.515K0.485]0.94Li0.06(Nb0.99Ta0.01)O3 (NKLNT) xMnO2yCuO (when x, y = 0, 0.005 and 0.01) were prepared by a reaction sintering method. The effects of doping level on sinterability and properties of NKLNT ceramics were studied. The results indicated that the co-doping of MnO2 and CuO was effective in promoting the densification of ceramics. Grain growth during secondary recrystallization was also affected, leading to larger grain size with x, y = 0.01 sample. X-ray diffraction data showed that the orthorhombic tetragonal morphotropic phase boundary existed in all the samples. At room temperature, the dielectric properties of NKLNT ceramics were improved by doping of appropriate MnO2 and CuO content. The temperature dependence of dielectric constant showed a decrease slightly in Curie temperature (TC) with increasing MnO2 and CuO content. The composition with x = 0.005, y = 0 exhibited favorable properties for the promising lead-free piezoelectric candidate material.