Accurate estimation of grassland leaf area index (LAI), fractional vegetation cover (FVC), and aboveground biomass (AGB) is fundamental in grassland studies. The newly launched Ocean and Land Color Imager (OLCI) sensor onboard Sentinel-3 (S3) provides images with comparable spatial and spectral resolution with MODIS data. However, the use of S3 OLCI imageries for vegetation variable estimation is rarely evaluated. This study evaluated the potential of S3 OLCI and MODIS data for estimating grassland LAI, FVC, and AGB in the eastern Eurasian steppe. A Bayesian spatial model (Integrated Nested Laplace Approximation with Stochastic Partial Differential Equation, INLA-SPDE) was used to address spatial autocorrelation of in-situ observation data and to enhance our predictions. Our results showed that the models based on S3 OLCI data presented higher accuracy than models with MODIS data. The RMSEs decreased by 3.7-10.8 %, 3.7-7.5 %, and 1.6-14.2 % for LAI, FVC, and AGB predictions, respectively. Through combinations of multiple predictors, we confirmed the robustness of red edge bands for grassland variable estimation, the models employing red edge variables yielded 3.5 %, 3.2 %, and 0.4 % lower RMSEs than models with conventional visible and NIR bands for LAI, FVC, and AGB prediction, respectively. INLA-SPDE spatial model produced lower bias and higher prediction accuracy than random forest and random forests kriging method in most of the models; the INLA-SPDE predicted LAI and FVC maps also showed a better agreement with ground observations than MODIS and PROBA-V land products.