In remote sensing applications, clouds are generally characterized by two properties: cloud optical thickness (COT) and effective radius of water–ice particles (Reff), as well as additionally by geometric properties when specific information is available. Most of the current operational passive remote sensing algorithms use a mono-angular bispectral method to retrieve COT and Reff. They are based on pre-computed lookup tables while assuming a homogeneous plane-parallel cloud layer. In this work, we use the formalism of the optimal estimation method, applied to airborne near-infrared high-resolution multi-angular measurements, to retrieve COT and Reff as well as the corresponding uncertainties related to the measurement errors, the non-retrieved parameters, and the cloud model assumptions. The measurements used were acquired by the airborne radiometer OSIRIS (Observing System Including PolaRization in the Solar Infrared Spectrum), developed by the Laboratoire d'Optique Atmosphérique. It provides multi-angular measurements at a resolution of tens of meters, which is very suitable for refining our knowledge of cloud properties and their high spatial variability. OSIRIS is based on the POLDER (POlarization and Directionality of the Earth's Reflectances) concept as a prototype of the future 3MI (Multi-viewing Multi-channel Multi-polarization Imager) planned to be launched on the EUMETSAT-ESA MetOp-SG platform in 2024. The approach used allows the exploitation of all the angular information available for each pixel to overcome the radiance angular effects. More consistent cloud properties with lower uncertainty compared to operational mono-directional retrieval methods (traditional bispectral method) are then obtained. The framework of the optimal estimation method also provides the possibility to estimate uncertainties of different sources. Three types of errors were evaluated: (1) errors related to measurement uncertainties, which reach 6 % and 12 % for COT and Reff, respectively, (2) errors related to an incorrect estimation of the ancillary data that remain below 0.5 %, and (3) errors related to the simplified cloud physical model assuming independent pixel approximation. We show that not considering the in-cloud heterogeneous vertical profiles and the 3D radiative transfer effects leads to an average uncertainty of 5 % and 4 % for COT and 13 % and 9 % for Reff.