The accurate estimation of suspended sediments (SSs) carries significance in determining the volume of dam storage, river carrying capacity, pollution susceptibility, soil erosion potential, aquatic ecological impacts, and the design and operation of hydraulic structures. The presented study proposes a new method for accurately estimating daily SSs using antecedent discharge and sediment information. The novel method is developed by hybridizing the multivariate adaptive regression spline (MARS) and the Kmeans clustering algorithm (MARS–KM). The proposed method’s efficacy is established by comparing its performance with the adaptive neuro-fuzzy system (ANFIS), MARS, and M5 tree (M5Tree) models in predicting SSs at two stations situated on the Yangtze River of China, according to the three assessment measurements, RMSE, MAE, and NSE. Two modeling scenarios are employed; data are divided into 50–50% for model training and testing in the first scenario, and the training and test data sets are swapped in the second scenario. In Guangyuan Station, the MARS–KM showed a performance improvement compared to ANFIS, MARS, and M5Tree methods in term of RMSE by 39%, 30%, and 18% in the first scenario and by 24%, 22%, and 8% in the second scenario, respectively, while the improvement in RMSE of ANFIS, MARS, and M5Tree was 34%, 26%, and 27% in the first scenario and 7%, 16%, and 6% in the second scenario, respectively, at Beibei Station. Additionally, the MARS–KM models provided much more satisfactory estimates using only discharge values as inputs.