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Chlorophyll-a (chl-a) is an important parameter of water quality and its concentration can be directly retrieved from satellite observations. The Ocean and Land Color Instrument (OLCI), a new-generation water-color sensor onboard Sentinel-3A and Sentinel-3B, is an excellent tool for marine environmental monitoring. In this study, we introduce a new machine learning model, Light Gradient Boosting Machine (LightGBM), for estimating time-series chl-a concentration in Fujian's coastal waters using multitemporal OLCI data and in situ data. We applied the Case 2 Regional CoastColour (C2RCC) processor to obtain OLCI band reflectance and constructed four spectral indices based on OLCI feature bands as supplementary input features. We also used root-mean-square error (RMSE), mean absolute error (MAE), median absolute percentage error (MAPE), and R2 as performance indicators. The results indicate that the addition of spectral indices can easily improve the prediction accuracy of the model, and normalized fluorescence height index (NFHI) has the best performance, with an RMSE of 0.38 µg/L, MAE of 0.22 µg/L, MAPE of 28.33%, and R2 of 0.785. Moreover, we used the well-known band ratio and three-band methods for chl-a estimation validation, and another two OLCI chl-a products were adopted for comparison (OC4Me chl-a and Inverse Modelling Technique (IMT) Neural Net chl-a). The results confirmed that the LightGBM model outperforms the traditional methods and OLCI chl-a products. This study provides an effective remote sensing technique for coastal chl-a concentration estimation and promotes the advantage of OLCI data in ocean color remote sensing. [ABSTRACT FROM AUTHOR]