As an emerging technology, virtual coupling improves the efficiency and flexibility of metro services by forming multiple trains (units) as a virtually coupled train set (VCTS) without mechanical couplers. However, to realize the desired VCTS operation in practical metro services, a significant gap to be filled is that the implicit and nonlinear safety constraints are hard to be addressed in real‐time control. Thus, this paper proposes a hierarchical control approach with a two‐layer framework. In the upper layer, a trajectory planning method is designed, which addresses the safety constraints and prescribes a reference trajectory for each unit. In the lower layer, a model predictive control approach is constructed, by which each unit accurately tracks its reference trajectory in real time. Afterward, the proposed hierarchical control approach is employed to realize VCTS inter‐station operation in field tests. The average tracking error of speed is around 8 cm/s and the stopping error is less than 12 cm. The following distance between two units in VCTS is reduced to less than 105 m at the speed of 80 km/h, which is a breakthrough in the development of VCTS.