This work investigates the regional climate and radiative effects of modifying surface albedo to mimic massive deployment of cool surfaces (roofs and pavements) and, separately, photovoltaic arrays across the United States. With the adoption of cool roofs and pavements, domain-wide annual average outgoing radiation increased by 0.16 ± 0.03 W m−2 (mean ± 95% C.I.) and afternoon summertime temperature in urban locations was reduced by 0.11–0.53 degrees Celsius, although some urban areas showed no statistically significant temperature changes. In response to increased urban albedo, some rural locations showed summer afternoon temperature increases of up to +0.27  degrees Celsius and these regions were correlated with less cloud cover and lower precipitation. The emissions offset obtained by this increase in outgoing radiation is calculated to be 3.3 ± 0.5 Gt CO2.