A new method for measuring the energy transfer upconversion (ETU) rate of laser crystal for solid-state lasers is provided in this paper. When the ETU effect is considered, the laser’s output power can be expressed in terms of the input power, the ETU rate and the nonradiative lifetime. Multiple sets of binary equations about the ETU rate and the nonradiative lifetime can be obtained by substituting the measured laser input–output powers into the equation of laser output power. By solving the binary equations, the ETU rate and the nonradiative lifetime of the laser crystal can be obtained simultaneously. Employing this method, the measured average values of ETU rate and nonradiative lifetime of the Nd:YLF (Nd3+, 1.0 at.%) crystal are 3.930 × 10−23 m3 s−1 and 6.274 × 10−3 s, respectively. The measured results are further analysed and discussed, showing the feasibility of the method. We believe that the proposed method can offer a good reference for measuring the ETU rate of new laser crystals.