NMC 811 has elicited great attention as a high energy cathode material for next generation lithium ion batteries. With 80% Ni content, NMC 811 has surpassed energy densities of previous generations of NMC cathodes. However, there exist inherent drawbacks to increasing nickel content, which limit the long-term cell performance. As compared to structurally similar NMCs, 811 suffers from poor cycle life and decreased stability due to the surface reactivity of now heightened nickel in the fully oxidized state. A number of surface-modification methods have been adopted to address these significant degradation issues including atomic layer deposition (ALD). ALD is a platform technology that has been widely demonstrated throughout the literature to impart significant processing and performance gains on lithium ion battery technologies, having notable impacts on surface stabilization of the positive electrode. In this work we will explore ALD as a means of controlling surface phenomena in cell architectures containing NMC 811, and present evidence for improved performance under high voltage conditions. In addition, we will demonstrate the synergistic effects of dually coated cells with significant enhancement resulting upon pairing ALD-enhanced 811 with surface-modified natural graphite. Alongside observations of high voltage stability, ALD-modified cells exhibit upwards of 30% increased cycle life and superior rate capabilities, increasing the attractiveness of this material for next generation LIBs.