Quantitative plant species α-diversity of grasslands at multiple spatial and temporal scales is important for investigating the responses of biodiversity to global change and protecting biodiversity under global change. Potential plant species α-diversity (i.e., SRp, Shannonp, Simpsonp and Pieloup: potential species richness, Shannon index, Simpson index and Pielou index, respectively) were quantified by climate data (i.e., annual temperature, precipitation and radiation) and actual plant species α-diversity (i.e., SRa, Shannona, Simpsona and Pieloua: actual species richness, Shannon index, Simpson index and Pielou index, respectively) were quantified by normalized difference vegetation index and climate data. Six methods (i.e., random forest, generalized boosted regression, artificial neural network, multiple linear regression, support vector machine and recursive regression trees) were used in this study. Overall, the constructed random forest models performed the best among the six algorithms. The simulated plant species α-diversity based on the constructed random forest models can explain no less than 96% variation of the observed plant species α-diversity. The RMSE and relative biases between simulated α-diversity based on the constructed random forest models and observed α-diversity were ≤1.58 and within ±4.49%, respectively. Accordingly, plant species α-diversity can be quantified from the normalized difference vegetation index and climate data using random forest models. The random forest models of plant α-diversity build by this study had enough predicting accuracies, at least for alpine grassland ecosystems, Tibet. The proposed random forest models of plant α-diversity by this current study can help researchers to save time by abandoning plant community field surveys, and facilitate researchers to conduct studies on plant α-diversity over a long-term temporal scale and larger spatial scale under global change.