Carbon dioxide capture and storage (CCS) is increasingly seen as a way for society to enjoy the benefits of fossil fuel energy sources while avoiding the climate disruption associated with fossil CO2 emissions. A decision to deploy CCS technology at scale should be based on robust information on its overall costs and benefits. Life-cycle assessment (LCA) is a framework for holistic assessment of the energy and environmental footprint of a system, and can provide crucial information to policy-makers, scientists, and engineers as they develop and deploy CCS systems. We identify seven key issues that should be considered to ensure that conclusions and recommendations from CCS LCA are robust: energy penalty, functional units, scale-up challenges, non-climate environmental impacts, uncertainty management, policy-making needs, and market effects. Several recent life-cycle studies have focused on detailed assessments of individual CCS technologies and applications. While such studies provide important data and information on technology performance, such case-specific data are inadequate to fully inform the decision making process. LCA should aim to describe the system-wide environmental implications of CCS deployment at scale, rather than a narrow analysis of technological performance of individual power plants.