To understand the long-term energy and climate implications of different implementation strategies for carbon capture and storage (CCS) in the US coal-fired electricity fleet, we integrate three analytical elements: scenario projection of energy supply systems, temporally explicit life cycle modeling, and time-dependent calculation of radiative forcing. Assuming continued large-scale use of coal for electricity generation, we find that aggressive implementation of CCS could reduce cumulative greenhouse gas emissions (CO2, CH4, and N2O) from the US coal-fired power fleet through 2100 by 37–58%. Cumulative radiative forcing through 2100 would be reduced by only 24–46%, due to the front-loaded time profile of the emissions and the long atmospheric residence time of CO2. The efficiency of energy conversion and carbon capture technologies strongly affects the amount of primary energy used but has little effect on greenhouse gas emissions or radiative forcing. Delaying implementation of CCS deployment significantly increases long-term radiative forcing. This study highlights the time-dynamic nature of potential climate benefits and energy costs of different CCS deployment pathways and identifies opportunities and constraints of successful CCS implementation.