The accuracy of model attitude measurement has an important impact on wind tunnel test results. Microelectromechanical System Inertial Measurement Unit (MEMS IMU) provides a feasible way to measure model attitudes with high accuracy. However, the installation error between MEMS IMU coordinate system and the body coordinate system of test models can make the accuracy of the model attitude measurement decrease. In wind tunnel tests, the installation error depends on the relationship between the IMU and the model mechanism before tests. Therefore, in-field calibration in wind tunnel tests is necessary to reduce installation errors. To improve attitude measurement accuracy, the least squares quaternion calibration method based on MEMS IMU and six-position calibration procedure are proposed. High-precision three-axis turntable tests are performed. The pitch accuracy after calibration is higher than that before calibration in the angle of attack sweeping tests. The Root-Mean-Square Errors (RMSE) in the roll and yaw are within 0.01°, which are smaller than those before calibration. In the roll sweeping tests, RMSE of three attitude angles decrease significantly. In hypersonic wind tunnel tests, the pitch errors before and after calibration are within 0.05° and 0.02° in the angle of attack sweeping tests without wind. In five angle of attack sweeping tests with wind, the deviation between the mean of the pitch and the pitch after the elastic angle correction is within 0.03° and the standard deviation of five tests is within 0.01°. The proposed method is confirmed to enhance the accuracy of attitude measurement effectively, which is convenient for engineering applications.