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Arm and hand function play a critical role in the successful completion of everyday tasks. Lost function due to neurological impairment impacts millions of lives worldwide. Despite improvements in the ability to assess and rehabilitate arm deficits, knowledge about underlying sources of impairment and related sequela remains limited. The comprehensive assessment of function requires the measurement of both biomechanics and neuromuscular contributors to performance during the completion of tasks that often use multiple joints and span three-dimensional workspaces. To our knowledge, the complexity of movement and diversity of measures required are beyond the capabilities of existing assessment systems. To bridge current gaps in assessment capability, a new exoskeleton instrument is developed with comprehensive bilateral assessment in mind. The development of the BiLateral Upper-limb Exoskeleton for Simultaneous Assessment of Biomechanical and Neuromuscular Output (BLUE SABINO) expands on prior iterations toward full-arm assessment during reach-and-grasp tasks through the development of a dual-arm and dual-hand system, with 9 active degrees of freedom per arm and 12 degrees of freedom (six active, six passive) per hand. Joints are powered by electric motors driven by a real-time control system with input from force and force/torque sensors located at all attachment points between the user and exoskeleton. Biosignals from electromyography and electroencephalography can be simultaneously measured to provide insight into neurological performance during unimanual or bimanual tasks involving arm reach and grasp. Design trade-offs achieve near-human performance in exoskeleton speed and strength, with positional measurement at the wrist having an error of less than 2 mm and supporting a range of motion approximately equivalent to the 50th-percentile human. The system adjustability in seat height, shoulder width, arm length, and orthosis width accommodate subjects from approximately the 5th-percentile female to the 95th-percentile male. Integration between precision actuation, human–robot-interaction force-torque sensing, and biosignal acquisition systems successfully provide the simultaneous measurement of human movement and neurological function. The bilateral design enables use with left- or right-side impairments as well as intra-subject performance comparisons. With the resulting instrument, the authors plan to investigate underlying neural and physiological correlates of arm function, impairment, learning, and recovery.