A major challenge for the estimation of crop traits (biophysical variables) from canopy reflectance is the creation of a high-quality training dataset. This can be addressed by using radiative transfer models (RTMs) to generate training dataset representing "real-world" data in situations with varying crop types and growth status as well as various observation configurations. However, this approach can lead to "ill-posed" problems related to assumptions in the sampling strategy and due to uncertainty in the model, resulting in unsatisfactory inversion results for retrieval of target variables. In order to address this problem, this research investigates a practical way to generate higher quality "synthetic" training data by integrating a crop growth model (CGM, in this case APSIM) with an RTM (in this case PROSAIL). This allows control of uncertainties of the RTM by imposing biological constraints on distribution and co-distribution of related variables. Subsequently, the method was theoretically validated on two types of synthetic dataset generated by PROSAIL or the coupling of APSIM and PROSAIL through comparing estimation precision for leaf area index (LAI), leaf chlorophyll content (Cab), leaf dry matter (Cm) and leaf water content (Cw). Additionally, the capabilities of current deep learning techniques using high spectral resolution hyperspectral data were investigated. The main findings include: (1) Feedforward neural network (FFNN) provided with appropriate configuration is a promising technique to retrieve crop traits from input features consisting of 1 nm-wide hyperspectral bands across 400-2500 nm range and observation configuration (solar and viewing angles), leading to a precise joint estimation for LAI (RMSE=0.061 m2 m-2), Cab (RMSE=1.42 μg cm-2), Cm (RMSE=0.000176 g cm-2) and Cw (RMSE=0.000319 g cm-2); (2) For the aim of model simplification, a narrower range in 400-1100 nm without observation configuration in input of FFNN model provided less precise estimation for LAI (RMSE=0.087 m2 m-2), Cab (RMSE=1.92 μg cm-2), Cm (RMSE=0.000299 g cm-2) and Cw (RMSE=0.001271 g cm-2); (3) The introduction of biological constraints in training datasets improved FFNN model performance in both average precision and stability, resulting in a much accurate estimation for LAI (RMSE=0.006 m2 m-2), Cab (RMSE=0.45 μg cm-2), Cm (RMSE=0.000039 g cm-2) and Cw (RMSE=0.000072 g cm-2), and this improvement could be further increased by enriching sample diversity in training dataset.