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Chlorophyll a and b content (Cab) and leaf area index (LAI) are two key parameters of crops, and their quantitative inversions are important for growth monitoring and the field management of wheat. However, due to the close correlation between the spectral signals of these two parameters and the effects of soil and atmospheric conditions, as well as modeling errors, synchronous retrieval of LAI and Cab from remote sensing data is still a challenging task. In a previous study, we introduced the optimal estimation theory and established the inversion framework by coupling the PROSAIL (PROSPECT + SAIL) model with the unified linearized vector radiative transfer model (UNL-VRTM). The framework fully utilizes the simulated radiance spectra for synchronous retrieval of Cab and LAI at the UAV observation scale and has good convergence and self-consistency. In this study, based on this inversion framework, synchronized retrieval of Cab and LAI was carried out by real wheat UAV observation data and validated with the ground-measured data. By comparing with the empirical statistical model constructed by the PROSAIL model and coupled model, least squares support vector machine (LSSVM), and random forest (RF), the proposed method has the highest accuracy of Cab and LAI estimated from UAV multispectral data (for Cab, R2 = 0.835, RMSE = 14.357; for LAI, R2 = 0.892, RMSE = 0.564). Our proposed method enables the fast and efficient estimation of Cab and LAI in multispectral data without prior measurements and training. [ABSTRACT FROM AUTHOR]