Grain storage has very strict temperature requirements. Aiming at the problems of nonlinear characteristics and poor prediction accuracy of temperature parameters in grain storage, a combination of chaos theory and enhanced radial basis neural network is proposed as a temperature prediction model for grain storage (C-ERBF). The model first determines the embedding dimension and time delay of the grain storage temperature sequence using chaos theory. It then calculates the Lyapunov exponent to confirm its chaotic properties and reconstructs the sequence in the phase space to extract the hidden dynamic information and structure behind the sequence. Furthermore, the q-Normalized Least Mean Square Fourth (qXE-NLMF) algorithm is designed to enhance the radial basis function (RBF) neural network model for weight updating, to improve its prediction accuracy, and to accelerate the training speed of the model. As verified by the simulation experiments of Mackey–Glass chaotic time series prediction, the enhanced RBF (ERBF) network has faster convergence speed and lower steady-state error compared to the traditional RBF network. Finally, the optimized dataset from chaos theory is input into the model to achieve accurate predictions of grain storage temperature series. The experimental results show that the proposed C-ERBF model has higher prediction accuracy compared to other time series prediction methods. It can realize the grain pile temperature in advance, and take control measures in advance. This proactive approach significantly reduces the consumption of stored grain and prevents issues before they arise.