Electrodynamic tethers can be employed as an immensely promising propulsion system for boosting the altitude of spacecraft, cite instance space stations, satellites, and the like, which ameliorates the expenditure of fuel and minimizes detrimental spacecraft impacts. This paper analyzes the libration dynamics and stability of reboost spacecraft with insulation electrodynamic tethers. A key aspect of spacecraft reboost with an electrodynamic tether is how to keep the tether aligned with the local vertical and stabilized in the context of external disturbances. It has been shown in the current research that the librational instability results in the tether slackness and swings in long-term motion without effective control. Moreover, electrodynamic force (Ampere force) is regarded as a distributed load acting on the tether causing tether deformations which may be detrimental if severe. Aiming at the problem, an optimal control method and PID are given to stabilize the libration motion by modulating the tether current. The dynamical model of the electrodynamic tether system is established using Lagrange equations of the second kind under considering tether deformation and control laws are proposed based on the model. The effectiveness of libration stability control is validated through numerical results in which a current regulation law with appropriate control parameters is used for the libration motion of electrodynamic tether system.