The tendency for movements of the upper limbs to be drawn systematically towards one another, and to follow similar spatiotemporal trajectories is well known. Although the suppression of this tendency is integral to tasks of daily living, its exploitation may prove to be critical in the rehabilitation of acquired hemiplegias. In general however, the task-related factors that determine the degree of coupling between the upper limbs, and the mechanisms that mediate bilateral interactions between neural pathways projecting to the muscles of the arm and hand, are not yet well understood. We present evidence that the postural context in which human participants perform upper limb movements, determines the relative stability of patterns of bimanual coordination. Manipulation of the axes of rotation of forearm movements reversed the relative stability of simultaneous and alternating patterns of bimanual coordination. Transcranial magnetic stimulation of motor cortex revealed that these manipulations of postural context altered the crossed-modulation of excitability in corticospinal pathways that arises from movement of the opposite limb. Furthermore, modulation of responses to electrical stimulation of the cervicomedullary junction indicated that crossed modulation was also expressed at the level of the spinal motoneurons. Our data support the view that crossed modulation of excitability in corticospinal pathways mediates the stability of bimanual coordination. Furthermore, task-related factors that are sufficient to give rise to changes in the stability of bimanual coordination are accompanied by crossed-modulation of excitability at multiple levels of the neuraxis, indicative of a failure of inhibitory control.