The optimization-based alignment (OBA) methods, which are implemented by the optimal attitude estimation using vector observations—also called double-vectors—have proven to be effective at solving the in-flight alignment (IFA) problem. However, the traditional OBA methods are not applicable for the low-cost strap-down inertial navigation system (SINS) since the error of double-vectors will be accumulated over time due to the substantial drift of micro-electronic- mechanical system (MEMS) gyroscope. Moreover, the existing optimal estimation method is subject to a large computation burden, which results in a low alignment speed. To address these issues, in this article we propose a new fast IFA method based on modified double-vectors construction and the gradient descent method. To be specific, the modified construction method is implemented by reducing the integration interval and identifying the gyroscope bias during the construction procedure, which improves the accuracy of double-vectors and IFA; the gradient descent scheme is adopted to estimate the optimal attitude of alignment without complex matrix operation, which results in the improvement of alignment speed. The effect of different sizes of mini-batch on the performance of the gradient descent method is also discussed. Extensive simulations and vehicle experiments demonstrate that the proposed method has better accuracy and faster alignment speed than the related traditional methods for the low-cost SINS/global positioning system (GPS) integrated navigation system