Electric vehicles powered by lithium-ion batteries are viewed as a vital green technology required to meet CO2 emission targets as part of a global effort to tackle climate change. Positive electrode (cathode) materials within such batteries are rich in critical metals—particularly lithium, cobalt, and nickel. The large-scale mining of such metals, to meet increasing battery demands, poses concerns surrounding material exhaustion in addition to further environmental, social, and governance (ESG) issues. In particular, unethical mining practices and political instability within the Democratic Republic of the Congo (the world's largest cobalt producer) have prompted research into cobalt-low and cobalt-free alternatives. This review aims to provide a holistic view of lithium-ion cathode development and inform advancements by highlighting the interdependencies across mining, material development, and end-of-life management. While material sustainability is reported through supply and demand projections, the potential socioenvironmental impacts of lithium-ion battery technology represent a hugely underresearched area among the aforementioned themes. Notably, the lack of attention paid toward future implications of increased nickel use across material management and development disciplines is also discussed.