In this paper, an autoregressive spectral estimation using a multilayered neural network is proposed to reduce the nonlinearities of 5G MIMO power amplifiers and increase the signal-transmitting qualities. The proposed method adopts the two-sided doubly exponential lattice algorithm to achieve the most suitable estimation for in-band compensation. Also, based on the iterative learning control method, a novel crest factor reduction digital predistortion is combined with the multilayered neural network. Based on the results, the proposed algorithm has increased the linearity and stability of the PA performance. The proposed method can improve the robustness of 5G MIMO wireless communication systems.