As Li-ion batteries continue to dominate in the portable electronics and electric car industries we look to increase capacity by cycling the batteries at higher voltages. Alloying transition metals and dopants to cathode materials can aid in pushing the voltage limit beyond current capabilities. However, at higher voltages, problems like interlayer dopant migration become a serious detriment that result in phase transformations and material break down. Using first-principles methods, we have unraveled the electronic structure that depresses interlayer atom migration. Surprisingly, this electronic structure is largely a contribution of the local environment around the dopant and not simply a function of the dopant’s identity. Using this understanding, we propose design principles for managing interlayer atom migration in cathode materials, with specific implications for NCA, NMC, and Li-excess cathodes.