Abstract: In geometrics, machine vision and other fields, the large rotation angle three-dimensional coordinate transformation often need to be applied based on the two corresponding point sets. The solvingmethods of the large rotation angle three-dimensional coordinate transformationare broadly divided into iterative methods and analytical methods. The iterative methods can obtain higher transformation accuracy. However, these methods depend on the initial value. In this contribution, quaternion is used to construct rotation matrix, a large rotation angle three-dimensional coordinate transformation formulae based on Newton iterative method is established, and a method which is widely used in guidance and control field for initial value calculation is given. Simulated and real data are used to validate the proposed algorithm, and the results are compared with those of other algorithms. The results show that the proposed algorithm makes the large rotation angle coordinate transformation model based on quaternion more robust. So the proposed algorithm is practically valuable for its stability of results, reliable accuracy and fast convergence.