In hydrological research, data assimilation (DA) is widely used to fuse the information contained in process‐based models and observational data to reduce simulation uncertainty. However, many popular DA methods are limited by low computational efficiency or their reliance on the Gaussian assumption. To address these limitations, we propose a novel DA method called DA(DL), which leverages the capabilities of DL to model non‐linear relationships and recognize complex patterns. DA(DL) first generates a large volume of training data from the prior ensemble, and then trains a DL model to update the system knowledge (e.g., model parameters in this study) from multiple predictors. For highly non‐linear models, an iterative form of DA(DL) can be implemented. Additionally, strategies of data augmentation and local updating are proposed to enhance DA(DL) for problems involving small ensemble size and the equifinality issue, respectively. In two hydrological DA cases involving Gaussian and non‐Gaussian distributions, DA(DL) shows promising performance compared to two ensemble smoother methods, that is, ES(K) and ES(DL), which respectively apply the Kalman‐ and DL‐based updates. Potential improvements to DA(DL) can be made by designing better DL model architectures, imposing physical constraints to the training of the DL model, and further updating other important variables like model states, forcings and error terms.