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With regards to the fourth stage rocket, upper stage flight time can be up to 48 hours. Volatile space environment leads parameters calibrated in ground do not meet the requirements of the spacecraft precise orbit. In this paper, a real-time on-orbit calibration method of redundant laser gyro inertial measurement unit for space transfer vehicle is proposed. We make use of the high precise attitude information from star sensor to design a calibration model with ten inertial instruments (five gyros and five accelerometers), which includes gyros drift, and scale factor error. The redundant gyros of strapdown inertial measurement unit parameters are estimated through Kalman filter and Sage-Husa adaptive filter. For this, we conduct numerical simulation. That the result of the parameters calibration precision is within 5% demonstrates the validity of this method on satisfying the navigation system's reliability and accuracy with the estimation and compensation for gyros error. The on-orbit calibration method provides a theoretical reference for the higher precise attitude determination of space transfer vehicle.