Leaf mass per area (LMA) and leaf equivalent water thickness (EWT) are key leaf functional traits providing information for many applications including ecosystem functioning modeling and fire risk management. In this paper, we investigate two common conclusions generally made for LMA and EWT estimation based on leaf optical properties in the near-infrared (NIR) and shortwave infrared (SWIR) domains: (1) physically-based approaches estimate EWT accurately and LMA poorly, while (2) statistically-based and machine learning (ML) methods provide accurate estimates of both LMA and EWT. Using six experimental datasets including broadleaf species samples of >150 species collected over tropical, temperate and boreal ecosystems, we compared the performances of a physically-based method (PROSPECT model inversion) and a ML algorithm (support vector machine regression, SVM) to infer EWT and LMA based on leaf reflectance and transmittance. We assessed several merit functions to invert PROSPECT based on iterative optimization and investigated the spectral domain to be used for optimal estimation of LMA and EWT. We also tested several strategies to select the training samples used by the SVM, in order to investigate the generalization ability of the derived regression models. We evidenced that using spectral information from 1700 to 2400¿nm leads to strong improvement in the estimation of EWT and LMA when performing a PROSPECT inversion, decreasing the LMA and EWT estimation errors by 55% and 33%, respectively. The comparison of various sampling strategies for the training set used with SVM suggests that regression models show limited generalization ability, particularly when the regression model is applied on data fully independent from the training set. Finally, our results demonstrate that, when using an appropriate spectral domain, the PROSPECT inversion outperforms SVM trained with experimental data for the estimation of EWT and LMA. Thus we recommend that estimation of LMA an