Surface metrology is an essential operation to determine whether the quality of manufactured surfaces meets the design requirements. In order to improve the surface accuracy and machining efficiency in the manufacturing of optical freeform surfaces, in-situ surface measurement without re-positioning the workpiece is considered as a promising technique in advanced manufacturing. In this study, a displacement laser scanner is integrated into an ultra-precision fly-cutting machine in order to perform as a coordinate measuring machine. However, some inevitable errors such as motion errors of the machine tool, thermal drift, vibrations, and errors of the laser sensor are introduced due to the manufacturing environment. To improve the performance of the measurement system, calibration of the main error sources is investigated with consideration of the characteristics of the built laser scanner system. Hence, the relationship between the moving speed of the laser scanner and the vibration of the tested signals is studied. Following that, the errors of the z-axis scale could be corrected by measuring a four-step heights artefact. Furthermore, volumetric positioning errors are identified by the proposed modified chi-square method and Gaussian processing prediction method. Simulation and measurement experiments are conducted, and the results indicate that the calibrated measuring system can measure ultra-precision freeform surfaces with micrometre form accuracy.