Neuroprosthetic systems based on functional electrical stimulation aim to restore motor function to individuals with paralysis following spinal cord injury. Identifying the optimal electrode set for the neuroprosthesis is complicated because it depends on the characteristics of the individual (such as injury level), the force capacities of the muscles, the movements the system aims to restore, and the hardware limitations (number and type of electrodes available). An electrode-selection method has been developed that uses a customized musculoskeletal model. Candidate electrode sets are created based on desired functional outcomes and the hard ware limitations of the proposed system. Inverse-dynamic simulations are performed to determine the proportion of target movements that can be accomplished with each set; the set that allows the most movements to be performed is chosen as the optimal set. The technique is demonstrated here for a system recently developed by our research group to restore whole-arm movement to individuals with high-level tetraplegia. The optimal set included selective nerve-cuff electrodes for the radial and musculocutaneous nerves; single-channel cuffs for the axillary, suprascapular, upper subscapular, and long-thoracic nerves; and muscle-based electrodes for the remaining channels. The importance of functional goals, hardware limitations, muscle and nerve anatomy, and surgical feasibility are highlighted.