Effective vibration control of flexible cables is increasingly demanded for space flexible structure. For the low frequency dynamics of flexible cables, a novel vibration control strategy based on sliding mode control is proposed in this paper. First, the complex dynamical behavior of flexible cables is modeled using D’Alembert’s principle. Second, an improved dual power reaching law is put forward to better address the chattering problem of the sliding mode controller. Then, an extended state observer (ESO) with the radial basis function (RBF) neural network is designed to compensate for internal uncertainties and external disturbances as well as further improve the control accuracy. Lyapunov function is employed to analyze the stability of the system. Finally, considering the large number of parameters of the proposed controller, an improved particle swarm optimization (PSO) algorithm is designed to automatically adjust these parameters. The effectiveness of the proposed method is demonstrated by simulation results.