Full waveform inversion (FWI) is a technique used to estimate subsurface model parameters by minimizing the difference between observed and calculated seismic data. Sparsity-promoting regularization are useful tools for traditional FWI methods to tackle complex subsurface structures. Since the traditional regularization techniques can only impose some fixed priors, it is necessary to develop a regularization strategy to obtain more flexible priors. In this way, we develop a structural sparse representation method that exploits the non-local self-similarity prior of the model, which is achieved by grouping similar patches using graph matching operators and a dynamic group selection strategy. A group-based dictionary is trained with the aim of providing the best sparse representation of complex features and variations in the entire model perturbation. The dynamic selection strategy of the training method can balance computational efficiency and inversion accuracy by constantly updating and retaining groups during the processing. In addition, two loop algorithm framework is utilized to enhance the robustness and the efficiency of the proposed method. Numerical experiments are presented to demonstrate that the proposed method outperforms the total variation regularization method and the adaptive dictionary learning with non-local self-similarity in terms of robustness and resolution. This structural sparsity-promoting regularization is incorporated into the FWI problem through a two-loop algorithm framework, enhancing the robustness and efficiency of FWI results.