Acousto-optic interaction geometry determines the spectral and spatial response of an acousto-optic tunable filter (AOTF). The precise calibration of the acousto-optic interaction geometry of the device is a necessary process before designing and optimizing optical systems. In this paper, we develop a novel calibration method based on the polar angular performance of an AOTF. A commercial AOTF device with unknown geometry parameters was experimentally calibrated. The experimental results show high precision, in some cases falling within 0.01°. In addition, we analyzed the parameter sensitivity and Monte Carlo tolerance of the calibration method. The results of the parameter sensitivity analysis show that the principal refractive index has a large influence on the calibration results, while other factors have little influence. The results of the Monte Carlo tolerance analysis show that the probability of the results falling 0.1° using this method is greater than 99.7%. This work provides an accurate and easy-to-perform method for AOTF crystal calibration and can contribute to the characteristic analysis of AOTFs and the optical design of spectral imaging systems.