On-orbit geometric calibration of satellite-borne laser based on infrared detectors is the key tool to ensure the elevation measurement accuracy, and the accuracy of on-orbit geometric calibration is directly determined by laser spots captured by detectors. Mathematical methods, such as gray-scale barycenter, are widely applied for centroid extraction of spots captured by infrared detectors and completely depend on the energy values at points measured by detectors, which have low precision and are greatly affected by the consistency of the detectors and other factors at present. Based on the above question, considering the consistency between the real laser footprint shape and spot captured by detectors, a centroid extraction method of laser spots captured by infrared detectors combining laser footprint images and detector observation data is proposed for making up this defect to some extent. First, the self-adaptive “two-step method” is used to denoise footprint images hierarchically to obtain the real shape of footprints for constraining the spots captured by detectors, and then the centroids of spots are extracted by using the energy-weighted barycenter method based on regional blocks. In the experiment, Gaofen-7 (GF-7) satellite is taken as the research object, and the proposed method, as well as the other six methods, are used for the centroid extraction of laser spots captured by detectors, the calculation of calibration parameters based on the single-beam and dual-beam laser calibration models, the positioning of laser footprints, and cross verification. According to the results, the plane accuracy of centroid extraction using the proposed method is as follows: 0.34 grids for Beam 1 and 0.33 grids for Beam 2. In addition, on flat terrain, the elevation accuracy of Beam 1 and Beam 2 in 2021 is 5.2 cm and 5.0 cm, respectively, 0.6 cm and 4.2 cm higher than those in the most accurate one among other methods; the elevation accuracy in 2020 is 23.3 cm and 7.1 cm, respectively, 7.7 cm and 2.7 cm higher than those in the most accurate one among other methods. On slopes and gentle slopes, the method proposed is also superior to other methods. Since the change of pointing angle caused by satellite jitter, atmosphere, etc., between different years, the accuracy drops when laser footprints of 2020 are located using the parameters of 2021. In summary, under different terrains and years, the results fully demonstrate the effectiveness and accuracy of the proposed method, which has more significant advantages than other traditional methods.