Optimal estimators are developed for computation of suspended-sediment concentrations in streams. The estimators are a function of parameters, computed by use of generalized least squares, which simultaneously account for effects of streamflow, seasonal variations in average sediment concentrations, a dynamic error component, and the uncertainty in concentration measurements. The parameters are used in a Kalman filter for on-line estimation and an associated smoother for off-line estimation of suspended-sediment concentrations. The accuracies of the optimal estimators are compared with alternative time-averaging interpolators and flow-weighting regression estimators by use of long-term daily-mean suspended-sediment concentration and streamflow data from 10 sites within the United States. For sampling intervals from 3 to 48 days, the standard errors of on-line and off-line optimal estimators ranged from 52.7 to 107%, and from 39.5 to 93.0%, respectively. The corresponding standard errors of linear and cubic-spline interpolators ranged from 48.8 to 158%, and from 50.6 to 176%, respectively. The standard errors of simple and multiple regression estimators, which did not vary with the sampling interval, were 124 and 105%, respectively. Thus, the optimal off-line estimator (Kalman smoother) had the lowest error characteristics of those evaluated. Because suspended-sediment concentrations are typically measured at less than 3-day intervals, use of optimal estimators will likely result in significant improvements in the accuracy of continuous suspended-sediment concentration records. Additional research on the integration of direct suspended-sediment concentration measurements and optimal estimators applied at hourly or shorter intervals is needed.