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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. Here 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 3/4 of the variability in clouds radiative cooling effect, 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 in present climate models. This hints to yet unknown compensating aerosol warming effects, possibly through deep clouds.