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• The Chla/TSS estimating algorithm was calibrated and validated for the Great Lakes. • Chla/TSS in the Great Lakes showed an increasing trend over the past 20 years. • The terrestrial input was an important reason for the variation in Chla/TSS. • Changes in Chla/TSS in western Lake Erie help predict the occurrence of blooms. Particulate composition provides important information for understanding the changes in underwater light fields and primary productivity. In this study, a semianalytical algorithm, based on Rayleigh-corrected reflectance at 678 nm and 748 nm on Moderate Resolution Imaging Spectroradiometer (MODIS) images was used to estimate the ratio of chlorophyll a to total suspended solids (Chla/TSS), which characterizes the particulate composition of the Great Lakes. The long-term spatial and temporal characteristics of Chla/TSS in the Great Lakes from 2000 to 2020 were obtained. The results demonstrated that Lake Superior had the highest average Chla/TSS values (5.79±0.76 µg/mg), while Lake Erie had the lowest average Chla/TSS values (2.93±0.76 µg/mg). The Mann-Kendall test showed that the Chla/TSS of the Great Lakes all showed an increasing trend, notably in Lake Michigan, with 88.23% pixels showing significant increasing trend. Climatic and hydrological factors dominated the intra-annual variation of Chla/TSS, with contribution rates ranging from 71.47% to 92.54%. Through the annual Chla/TSS change pattern analysis, it was found that the contribution of wind speed to the annual variation in Chla/TSS was slight. Changes in temperature played a major role in the interannual variability of Chla/TSS in Lake Superior and Ontario; runoff and settlement were the major contributors in Lake Huron and Michigan, while cropland dominated the Chla/TSS interannual variability in Lake Erie. Furthermore, the significantly low values of Chla/TSS in spring had the potential to predict the occurrence of blooms in western Lake Erie, and the spatial distribution of Chla/TSS could help predict the location of blooms in the next few days. [Display omitted] [ABSTRACT FROM AUTHOR]