A lack of reliable estimates of cloud condensation nuclei (CCN) aerosols over oceans has severely limited our ability to quantify their effects on cloud properties and extent of cooling by reflecting solar radiation-a key uncertainty in anthropogenic climate forcing. We introduce a methodology for ascribing cloud properties to CCN and isolating the aerosol effects from meteorological effects. Its application showed that for a given meteorology, CCN explains three-fourths of the variability in the radiative cooling effect of clouds, mainly through affecting shallow cloud cover and water path. This reveals a much greater sensitivity of cloud radiative forcing to CCN than previously reported, which means too much cooling if incorporated into present climate models. This suggests the existence of compensating aerosol warming effects yet to be discovered, possibly through deep clouds.