Harmony is a bimanual upper-limb exoskeleton designed for post-stroke rehabilitation. It moves the subject's shoulders and arms through their entire ranges of motion while maintaining natural coordination, is capable of force/torque control of each joint, and is equipped with sensors to measure motions and interaction forces. With these capabilities Harmony has the potential to assess motor function and create individualized therapy regimens. As a first step, five stroke survivors underwent rehabilitation sessions practicing multijoint movements with the device. Each participant performed a total of 1130 motions over seven hours of therapy with no adverse effects reported by participants or the attending therapist, supporting the suitability of Harmony for use in a clinical setting. Donning and doffing time averaged 3.5 minutes and decreased with therapist experience. Reported levels of stress, anxiety, and pain indicate that the Harmony safely assisted in the completion of the trained movements and has great potential to motivate and engage patients. We developed a novel methodology for assessing coordination capability and results from the study indicate that Harmony can enable therapists to identify neuromuscular weakness and maladaptive coordination patterns and develop targeted interventions to address these aspects of upper-limb function. The results suggest Harmony's feasibility and show promising improvements, motivating future study to gain statistical support.