The assessment and diagnosis of controller performance for model‐based closed‐loop control systems has received considerable attention in recent years. A recognized factor dilapidating the controller performance is mismatching the true dynamical model of the plant and the mathematic model employed in the controller. In order to reduce the heavy effort to re‐identify the entire model, a large amount of recent works have been focusing on locating the mismatch. To further improve the mathematic model as well as controller performance, in this article, we provide a novel prediction‐based plant‐model mismatch quantification approach, which belongs to the class of moment match methodology. In particular, two cases of output prediction are considered: one‐step ahead prediction and multistep ahead prediction. Compared with existing efforts along the same line of mismatch quantification, when using the one‐step ahead prediction, our method shows an advantage of light computational complexity. On the other hand, when utilizing multistep predictions, it shows better convergence and robustness than the former, especially in the case of structural mismatches, and the long‐term prediction capability of the model is employed. With both predictions and consideration of the existence of unknown noise models in practice, we show that the plant‐model mismatch and unknown parameters of noise models can be quantified as the solution of a minimization issue that penalizes the discrepancy between the sample of plant outputs and the predictions calculated by considering the plant‐model mismatch and noise model parameters. Several examples are provided to demonstrate the effectiveness of the proposed methods, respectively.