Freeform surface is one of the research focuses in the measurement field. A composite module is composed of a plane and rotating paraboloid. The composite module array can identify 21 geometric errors of the machine tool in a wide range, which is composed of several composite modules. Eliminating the error of the array itself is of great significance for improving measurement accuracy. For this reason, this paper proposed a noncontact method for calibrating the angle and position of the composite module array. This paper used a self-developed angle sensor to access corresponding information and established the mathematical model according to the freeform surface’s geometric characteristics to achieve calibration. In addition, the influence of array placement error on calibration was analyzed. The experimental results showed that the angle repeatability was within 0.4″ around the X-axis and within 0.3″ around the Y-axis, and the position repeatability was within 0.4 µm in the X direction and within 0.7 µm in the Y direction. The measurement comparison experiments with high-precision laser interferometer and uncalibrated array verified the correctness of the experimental results. This method provides an important reference for practical application and freeform surface array calibration, and creates conditions for the implementation of machine tool error detection.