Background: The growing health risks associated with greenhouse gas emissions highlight the need for new energy policies that emphasize efficiency and low-carbon energy intensity. Objectives: We assessed the relationships among electricity use, coal consumption, and health outcomes. Methods: Using time-series data sets from 41 countries with varying development trajectories between 1965 and 2005, we developed an autoregressive model of life expectancy (LE) and infant mortality (IM) based on electricity consumption, coal consumption, and previous year's LE or IM. Prediction of health impacts from the Greenhouse Gas and Air Pollution Interactions and Synergies (GAINS) integrated air pollution emissions health impact model for coal-fired power plants was compared with the time-series model results. Results: The time-series model predicted that increased electricity consumption was associated with reduced IM for countries that started with relatively high IM (> 100/1,000 live births) and low LE (< 57 years) in 1965, whereas LE was not significantly associated with electricity consumption regardless of IM and LE in 1965. Increasing coal consumption was associated with increased IM and reduced LE after accounting for electricity consumption. These results are consistent with results based on the GAINS model and previously published estimates of disease burdens attributable to energy-related environmental factors, including indoor and outdoor air pollution and water and sanitation. Conclusions: Increased electricity consumption in countries with IM < 100/1,000 live births does not lead to greater health benefits, whereas coal consumption has significant detrimental health impacts.