Various promising applications of electrodynamic tether have been proposed for space missions over the past decades. A crucial issue of these missions is to deploy an electrodynamic tether under a rapid and stable state. This paper aims to stabilize the libration motions of a bare electrodynamic tether during its three-dimensional deployment. The tethered system under consideration consists of a main-satellite and a sub-satellite connected to each other through a bare electrodynamic tether. A widely used dumbbell assumption considering the tether as rigid and inflexible is adopted to facilitate the dynamic modeling and analysis of the tethered system. A pair of active control laws is synthesized by simultaneously regulating the electric current and tether tension to achieve an efficient stabilization of the three-dimensional libration of the bare electrodynamic tether in the deployment process.