Kinetic characteristics of Li+ intercalation/deintercalation into/from individual LiNi0.8Co0.15Al0.05O2 particles in a composite cathode were studied in situ using Raman microscopy during galvanostatic charge-discharge in 1.2 M LiPF6, ethylene carbonate (EC): ethyl methyl carbonate (EMC), 3:7 by volume. Ex situ spectroscopic analysis of a cathode that was removed from a tested high-power Li-ion cell, which suffered substantial power and capacity loss, showed that the state of charge (SOC) of oxide particles on the cathode surface was highly nonuniform despite deep discharge of the Li-ion cell at the end of the test. In situ monitoring of the SOC of selected oxide particles in the composite cathode in a sealed spectro-electrochemical cell revealed that the rate at which particles charge and discharge varied with time and location. The inconsistent kinetic behavior of individual oxide particles was attributed to degradation of the electronically conducting carbon matrix in the composite cathode upon testing. These local microphenomena are most likely responsible for the overall impedance rise of the cathode and contribute to the mechanism of lithium-ion cell failure.