How to accurately identify unknown time-varying external force from measured structural responses is an important engineering problem, which is critical for assessing the safety condition of the structure. In the context of a few available accelerometers, this paper proposes a novel time-varying external force identification method using group sparse regularization based on the prior knowledge in the redundant dictionary. Firstly, the relationship between time-varying external force and acceleration responses is established, and a redundant dictionary is designed to create a sparse expression of external force. Then, the relevance of atoms in the redundant dictionary is revealed, and this prior knowledge is used to determine the group structures of atoms. As a result, a force identification governing equation is formulated, and the group sparse regularization is reasonably introduced to ensure the accuracy of the identified results. The contribution of this paper is that the group structures of atoms are reasonably determined based on prior knowledge, and the complexity in the process for identifying external force from measured acceleration responses is reduced. Finally, the effectiveness of the proposed method is demonstrated by numerical simulations and an experimental structure. The illustrated results show that, compared with the force identification method based on the standard l1-norm regularization, the proposed method can further improve the identified accuracy of unknown external force and greatly enhance the computational efficiency for the force identification problem.