Abstract. A cloud–aerosol–radiation (CAR) ensemble modeling system has been developed to incorporate the largest choices of alternate parameterizations for cloud properties (cover, water, radius, optics, geometry), aerosol properties (type, profile, optics), radiation transfers (solar, infrared), and their interactions. These schemes form the most comprehensive collection currently available in the literature, including those used by the world's leading general circulation models (GCMs). CAR provides a unique framework to determine (via intercomparison across all schemes), reduce (via optimized ensemble simulations), and attribute specific key factors for (via physical process sensitivity analyses) the model discrepancies and uncertainties in representing greenhouse gas, aerosol, and cloud radiative forcing effects. This study presents a general description of the CAR system and illustrates its capabilities for climate modeling applications, especially in the context of estimating climate sensitivity and uncertainty range caused by cloud–aerosol–radiation interactions. For demonstration purposes, the evaluation is based on several CAR standalone and coupled climate model experiments, each comparing a limited subset of the full system ensemble with up to 896 members. It is shown that the quantification of radiative forcings and climate impacts strongly depends on the choices of the cloud, aerosol, and radiation schemes. The prevailing schemes used in current GCMs are likely insufficient in variety and physically biased in a significant way. There exists large room for improvement by optimally combining radiation transfer with cloud property schemes.