The closed-form solution of circular membranes subjected to gas pressure loading plays an extremely important role in technical applications such as characterization of mechanical properties for freestanding thin films or thin-film/substrate systems based on pressured bulge or blister tests. However, the only two relevant closed-form solutions available in the literature are suitable only for the case where the rotation angle of membrane is relatively small, because they are derived with the small-rotation-angle assumption of membrane, that is, the rotation angle θ of membrane is assumed to be small so that “sinθ = 1/(1 + 1/tan2θ)1/2” can be approximated by “sinθ = tanθ”. Therefore, the two closed-form solutions with small-rotation-angle assumption cannot meet the requirements of these technical applications. Such a bottleneck to these technical applications is solved in this study, and a new and more refined closed-form solution without small-rotation-angle assumption is given in power series form, which is derived with “sinθ = 1/(1 + 1/tan2θ)1/2”, rather than “sinθ = tanθ”, thus being suitable for the case where the rotation angle of membrane is relatively large. This closed-form solution without small-rotation-angle assumption can naturally satisfy the remaining unused boundary condition, and numerically shows satisfactory convergence, agrees well with the closed-form solution with small-rotation-angle assumption for lightly loaded membranes with small rotation angles, and diverges distinctly for heavily loaded membranes with large rotation angles. The confirmatory experiment conducted shows that the closed-form solution without small-rotation-angle assumption is reliable and has a satisfactory calculation accuracy in comparison with the closed-form solution with small-rotation-angle assumption, particularly for heavily loaded membranes with large rotation angles.