For high-dimensional closed quantum systems, this paper proposes a novel quantum Lyapunov control scheme based on the particle swarm optimization algorithm and achieves a high-probability population transfer of the system to a non-isolated target eigenstate in the LaSalle invariant set under usual smooth Lyapunov control laws. Via a quadratic Lyapunov function with unknown parameters, a control law with the unknown parameters is designed; based on the LaSalle invariance principle and the energylevel connectivity graph, the stability of the system is analyzed; by using the particle swarm optimization algorithm, a set of optimal parameters is obtained to achieve the control goal. In particular, we propose a path planning method based on the energy-level connectivity graph to determine the initial values of the unknown parameters, which is such that the optimization algorithm can efficiently and conveniently find a set of optimal solutions of the unknown parameters. Numerical simulation experiments on a five-level quantum system and a three-qubit system demonstrate that the proposed Lyapunov control scheme based on the particle swarm optimization algorithm has a good control effect. INDEX TERMS High-dimensional quantum systems, Lyapunov control, particle swarm optimization algorithm, parameter optimization, initial values, energy-level connectivity graph.