Chlorophyll a concentration is an important indicator to characterize phytoplankton biomass, which further reflects the water quality of lakes. Based on the data of chlorophyll a concentration and environmental factors extracted from the ChlaData, HydroLAKES, and HELLAKES databases for Chinese lakes for three years (2000, 2005, and 2010), we used the random forest model and the generalized linear model to analyze the relationship between chlorophyll a concentration and environmental factors in Chinese lakes and predict the chlorophyll a concentration. The results showed that the relative importance of environmental factors for chlorophyll a was as follows: nutrient salt concentration > longitude and latitude > monthly mean precipitation > altitude > annual average temperature. The coefficient of determination of the random forest model was 0.9997 (R2 = 0.9997), and the root-mean-square error was 0.0010 (RMSE = 0.0010), with high prediction accuracy. The random forest model and the generalized linear model both showed that TP was the main influencing factor of chlorophyll a concentration. The validation results based on the measured data show that the models are reliable. By making more accurate predictions of chlorophyll a concentrations, we can facilitate the prevention, control, and treatment of lake blooms.