Systematic errors generated from internal misalignments of a lab-built terrestrial laser scanner (TLS) need to be calibrated to improve the positional accuracy of point-cloud. Hence, an angle measurement error model was established by the ray-tracing method involving five types of mounting angle errors, which were estimated by two-face method and network method. Experimental results show that the two errors including mirror tilt error and vertical index offset error are regarded as main systematic errors for lab-built TLS, and consequently the positional accuracy of the point-cloud can be improved in horizontal and vertical directions. The proposed self-calibration method can be used for other TLS by adjusting the angle measurement error model.