As an ideal calibration source, the moon has stable spectral characteristics and light intensity within the dynamic range of the detector. Thus, lunar calibration on-orbit is one of the important means to improve the efficiency of radiometric calibration and monitor the imaging stability of remote sensing satellites. Targeting low earth orbit and high-resolution remote sensing satellites, an on-orbit lunar calibration method, which includes imaging time, satellite attitude, imaging parameters of lunar observation, etc., is proposed in this paper. Lunar observation experiments on a low-orbit optical remote sensing satellite were successfully conducted 15 times in July, 2019, under the conditions of satellite attitude angular velocity of 0.06 (°)/s and integration time of 0.293 8 ms. The lunar phase angle covered the range of -79.872° to 89.236°. The results suggest that the satellite attitude of the actual implementation is in accordance with that of the design. Moreover, the lunar calibration method has high observation efficiency, which takes only 1 500 s and will not affect the normal earth observation mission. Furthermore, the texture of 15 acquired images of the moon has a better distribution hierarchy of image DN value, and the spatial resolution is better than 1.18 km. The calculated lunar irradiance distribution trend is consistent with that of the RObotic Lunar Observatory (ROLO) model published internationally. The experimental results verified the correctness and rationale of the proposed method. Multiple lunar phase angle observation has been realized for the first time in China though the attitude maneuver of a low-orbit remote sensing satellite, which can provide a reliable basis for long-term monitoring of the imaging stability of the senor and accumulating a large amount of lunar calibration data to establish a lunar radiation model independently in China.