Chaotic time series are widely present in practice, but due to their characteristics—such as internal randomness, nonlinearity, and long-term unpredictability—it is difficult to achieve high-precision intermediate or long-term predictions. Multi-layer perceptron (MLP) networks are an effective tool for chaotic time series modeling. Focusing on chaotic time series modeling, this paper presents a generalized degree of freedom approximation method of MLP. We then obtain its Akachi information criterion, which is designed as the loss function for training, hence developing an overall framework for chaotic time series analysis, including phase space reconstruction, model training, and model selection. To verify the effectiveness of the proposed method, it is applied to two artificial chaotic time series and two real-world chaotic time series. The numerical results show that the proposed optimized method is effective to obtain the best model from a group of candidates. Moreover, the optimized models perform very well in multi-step prediction tasks.