This paper proposes a two-level hierarchical control approach based on pursuit-evasion game and mean field game for the problem of large-scale pursuers with multi-population against a single evader, which implements that the evader is surrounded by pursuers. At the upper layer, we model the pursuit-evasion game between the centers of the pursuer populations and the single evader, which is formulated as a linear quadratic differential game (LQDG) to obtain the optimal control of each player. Then the optimal trajectories derived from the optimal controls are input to the lower layer as the reference trajectories. At the lower layer, we formulate the tracking of reference trajectories and terminal surrounding to the evader of large-scale pursuers with multi-population as a multi-population mean-field game (MPMFG), which solves the communication and computing difficulties caused by large-scale agents. Then, we derive the variational primal–dual formulation of the proposed MPMFG model and solve it with CA-Net, a coupled alternating neural network approach. Finally, simulation experiments are performed under various pursuit-evasion scenarios, and it is verified that the proposed game-based two-level hierarchical control approach is feasible and effective.