Thermal radiation induced by NIR laser, from rare earth doped oxides show promising potentials in many applications, due to their relatively high luminescent efficieny in the visible light region. Therefore, further enhancing the efficiency of this type of thermal radiation is of vital importance. In this paper, we proposed a protocol to improve the luminescent efficiency of the thermal radiation, that is, introducing Li+ into the oxide hosts, which on one hand could decrease the symmetry around the rare earth ions, and on the other, could create the inner defects due to the mismatch of valences. Beneficial effects of doping Li+ including the enhancement of the absorption of rare earth ions at the incident wavelength (due to the enhanced crystal field), as well as the promotion of producing heat associated with lattice phonons (owing to the increased so called “luminescence quechers”). In addition, we synthesized series of Li+ and Yb3+ doped ZrO2 using sol-gel technique to experimentally validate our proposed design, influences of doping Li ions on the structure of the nnaocrystals were discussed on the basis of XRD and TEM tests; through the emission spectra, the effects of doping concentration were investigated as well. This work may provide references for fabricating oxide phosphors with efficient thermal radiation.