The Gao Fen Xiang Ji (GFXJ) is the first Chinese self–developed airborne three–line array charge-coupled devices (CCD) camera and is designed to meet 8 cm ground sample distance (GSD), 0.5 m planimetry accuracy, and 0.28 m elevation accuracy for ground three-dimensional (3D) points at a flight height of 2000 m. These values also meet the 1:1000 scale mapping requirements in China. However, the original direct geopositioning accuracy of the GFXJ is approximately 4 m in the planimetry direction and 6 m in the elevation direction. To meet the ground 3D point accuracy requirements and improve the direct geopositioning accuracy of the GFXJ, this paper carries out a deep investigation on the GFXJ geometric calibration. This geometric calibration includes two main parts: the Global Navigation Satellite System (GNSS) lever arms and inertial measurement unit (IMU) boresight misalignment calibration, and the camera lens and CCD line distortion calibration. First, a brief introduction is given on the imaging properties of the GFXJ camera. Then, the GNSS lever arms and IMU boresight misalignment calibration models are built for the GFXJ camera. Next, a piecewise self-calibration model based on the CCD viewing angle is established for the GFXJ lens and CCD line distortion calibration. Subsequently, an iterative two-step calibration scheme is proposed for the geometric calibration. Finally, experiments were implemented using multiple flight blocks obtained in the Songshan remote sensing comprehensive field and the Hegang area of Heilongjiang Province. Through calibration experiments, geometric calibration values were obtained for the GNSS lever arms and IMU boresight misalignment. Reliable CAM files were independently generated for the forward, nadir, and backward line arrays. The experiments showed that the proposed GNSS lever arms and IMU boresight misalignment calibration models and the piecewise self-calibration model had good applicability and effectiveness for the GFXJ camera. The proposed two-step calibration scheme can significantly enhance the geometric positioning accuracy of the GFXJ camera. The original direct geopositioning accuracy of the GFXJ is approximately 4 m in the planimetry direction and 6 m in the elevation direction. Using the GNSS lever arms and the IMU boresight misalignment calibration values and the CAM files, the positioning accuracy of the GFXJ camera can fulfill the 3D point accuracy requirements and the 1:1000 mapping accuracy requirements at a 2000 m flight height after aerial triangulation with only several ground control points. The planimetry accuracy is approximately 0.2 m, and the elevation accuracy is less than 0.28 m. In addition, the calibration models and calibration scheme established in this paper can provide a reference for calibration studies on other airborne linear array CCD cameras.