Overcharge of lithium-ion batteries can lead to the deposition of lithium ions on the surface of graphite electrodes. The phenomenon of lithium deposition causes reduced electrochemical performance and presents safety concerns for lithium-ion batteries in high-power applications. This study presents a technique using neutron radiography (NR) for in situ visualization of the effects of overcharge in a graphite/NCA (LiNi0.8Co0.15Al0.05O2) lithium-ion cell. Patterns of deposition of solid material on the surface of the graphite electrode observed in the radiographs were confirmed by direct observation of the electrode. Inductively coupled plasma mass spectrometry was used to verify the elemental contents of the deposited material. NR is shown to be a promising tool for the study of lithium-ion batteries in high-power applications.