Longwave (LW) spectral flux and cloud radiative effect (CRE) are important for understanding the earth’s radiation budget and cloud–radiation interaction. Here, the authors extend their previous algorithms to collocated Atmospheric Infrared Sounder (AIRS) and Cloud and the Earth’s Radiant Energy System (CERES) observations over the entire globe and show that the algorithms yield consistently good performances for measurements over both land and ocean. As a result, the authors are able to derive spectral flux and CRE at 10-cm21 intervals over the entire LW spectrum from all currently available collocated AIRS and CERES observations. Using this multiyear dataset, they delineate the climatology of spectral CRE, including the far IR, over the entire globe as well as in different climate zones. Furthermore, the authors define two quantities, IR-effective cloud-top height (CTHeff) and cloud amount (CAeff), based on the monthly-mean spectral (or band by band) CRE. Comparisons with cloud fields retrieved by the CERES–Moderate Resolution Imaging Spectroradiometer (MODIS) algorithm indicate that, under many circumstances, the CTHeff and CAeff can be related to the physical retrievals of CTH and CA and thus can enhance understandings of model deficiencies in LW radiation budgets and cloud fields. Using simulations from the GFDL global atmosphere model, version 2 (AM2); NASA’s Goddard Earth Observing System, version 5 (GEOS-5); and Environment Canada’s Canadian Centre for Climate Modelling and Analysis (CCCma) Fourth Generation Canadian Atmospheric General Circulation Model (CanAM4) as case studies, the authors further demonstrate the merits of the CTHeff and CAeff concepts in providing insights on global climate model evaluations that cannot be obtained solely from broadband LW flux and CRE comparisons.