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UAV (unmanned aerial vehicle) remote sensing provides the feasibility of high-throughput phenotype nondestructive acquisition at the field scale. However, accurate remote sensing of crop physicochemical parameters from UAV optical measurements still needs to be further studied. For this purpose, we put forward a crop phenotype inversion framework based on the optimal estimation (OE) theory in this paper, originating from UAV low-altitude hyperspectral/multispectral data. The newly developed unified linearized vector radiative transfer model (UNL-VRTM), combined with the classical PROSAIL model, is used as the forward model, and the forward model was verified by the wheat canopy reflectance data, collected using the FieldSpec Handheld in Qi County, Henan Province. To test the self-consistency of the OE-based framework, we conducted forward simulations for the UAV multispectral sensors (DJI P4 Multispectral) with different observation geometries and aerosol loadings, and a total of 801 sets of validation data were obtained. In addition, parameter sensitivity analysis and information content analysis were performed to determine the contribution of crop parameters to the UAV measurements. Results showed that: (1) the forward model has a strong coupling between vegetation canopy and atmosphere environment, and the modeling process is reasonable. (2) The OE-based inversion framework can make full use of the available radiometric spectral information and had good convergence and self-consistency. (3) The UAV multispectral observations can support the synchronous retrieval of LAI (leaf area index) and Cab (chlorophyll a and b content) based on the proposed algorithm. The proposed inversion framework is expected to be a new way for phenotypic parameter extraction of crops in field environments and had some potential and feasibility for UAV remote sensing. [ABSTRACT FROM AUTHOR]