Fractional derivatives and regime-switching models are widely used in various fields of finance because they can describe the nonlocal properties of the solutions and the changes in the market status, respectively. The regime-switching time-fractional diffusion equations that combine both advantages are also used in European option pricing; however, to our knowledge, American option pricing based on such models and their numerical methods is yet to be studied. Hence, a fast algorithm for solving the multi-state time-fractional linear complementary problem arising from the regime-switching time-fractional American option pricing models is developed in this paper. To construct the solution strategy, the original problem has been converted into a Hamilton–Jacobi–Bellman equation, and a nonlinear finite difference scheme has been proposed to discretize the problem with stability analysis. A policy-Krylov subspace method is developed to solve the nonlinear scheme. Further, to accelerate the convergence rate of the Krylov method, a tri-diagonal preconditioner is proposed with condition number analysis. Numerical experiments are presented to demonstrate the validity of the proposed nonlinear scheme and the efficiency of the proposed preconditioned policy-Krylov subspace method.