This work presents a non-destructive in-situ method for probing degradation mechanisms in large format, operating, commercial lithium-ion batteries by neutron diffraction. A fresh battery (15 Ah capacity) was shown to have a uniform (homogeneous) local state of charge (SOC) at 4.0 V (9 Ah SOC) and 4.2 V (15 Ah SOC), with 1.33 C and 2.67 C charging rates, respectively. This battery was then aggressively cycled until it retained only a 9 Ah capacity, 60% of its original value. Inhomogeneous deterioration in the battery was observed: near the edges, both the graphite anode and the spinel-based cathode showed a significant loss of capacity, while near the central area, both electrodes functioned properly. An SOC mapping measurement of the degraded battery in the fully charged state (4.2 V) indicated that the loss of local capacity of the anode and cathode is coupled. (C) 2013 Elsevier B.V. All rights reserved.