A computationally efficient high-spectral-resolution cloudy-sky radiative transfer model (HRTM) in the thermal infrared region (700–1300 cm21, 0.1 cm21 spectral resolution) is advanced for simulating the upwelling radiance at the top of atmosphere and for retrieving cloud properties. A precomputed transmittance database is generated for simulating the absorption contributed by up to seven major atmospheric absorptive gases (H2O, CO2, O3, O2, CH4, CO, and N2O) by using a rigorous line-by-line radiative transfer model (LBLRTM). Both the line absorption of individual gases and continuum absorption are included in the database. A high-spectral-resolution ice particle bulk scattering properties database is employed to simulate the radiation transfer within a vertically nonisothermal ice cloud layer. Inherent to HRTM are sensor spectral response functions that couple with high-spectral-resolution measurements in the thermal infrared regions from instruments such as the Atmospheric Infrared Sounder (AIRS) and Infrared Atmospheric Sounding Interferometer. When compared with the LBLRTM and the discrete ordinates radiative transfer model (DISORT), the root-mean-square error of HRTM-simulated single-layer cloud brightness temperatures in the thermal infrared window region is generally smaller than 0.2 K. An ice cloud optical property retrieval scheme is developed using collocated AIRS and Moderate Resolution Imaging Spectroradiometer (MODIS) data. A retrieval method is proposed to take advantage of the high-spectral-resolution instrument. On the basis of the forward model and retrieval method, a case study is presented for the simultaneous retrieval of ice cloud optical thickness t and effective particle size Deff that includes a cloud-top-altitude self-adjustment approach to improve consistency with simulations.