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The in-flight alignment is a critical stage for airborne inertial navigation system/Global Positioning System (INS/GPS) applications. The alignment task is usually carried out by the Kalman filtering technique that necessitates a good initial attitude to obtain a satisfying performance. Due to the airborne dynamics, the in-flight alignment is much more difficult than the alignment on the ground. An optimization-based coarse alignment approach that uses GPS position/velocity as input, founded on the newly-derived velocity/position integration formulae is proposed. Simulation and flight test results show that, with the GPS lever arm well handled, it is potentially able to yield the initial heading up to 1 deg accuracy in 10 s. It can serve as a nice coarse in-flight alignment without any prior attitude information for the subsequent fine Kalman alignment. The approach can also be applied to other applications that require aligning the INS on the run.