Methylmercury is a global pollutant of aquatic ecosystems, and monitoring programs need tools to predict mercury exposure of wildlife. We developed equations to estimate methylmercury exposure of piscivorous birds and sport fish using mercury concentrations in prey fish. We collected original data on western grebes (Aechmophorus occidentalis) and Clark’s grebes (Aechmophorus clarkii) and summarized the published literature to generate predictive equations specific to grebes and a general equation for piscivorous birds. We measured mercury concentrations in 354 grebes (blood averaged 1.06 ± 0.08 μg/g ww), 101 grebe eggs, 230 sport fish (predominantly largemouth bass and rainbow trout), and 505 prey fish (14 species) at 25 lakes throughout California. Mercury concentrations in grebe blood, grebe eggs, and sport fish were strongly related to mercury concentrations in prey fish among lakes. Each 1.0 μg/g dw (∼0.24 μg/g ww) increase in prey fish resulted in an increase in mercury concentrations of 103% in grebe blood, 92% in grebe eggs, and 116% in sport fish. We also found strong correlations between mercury concentrations in grebes and sport fish among lakes. Our results indicate that prey fish monitoring can be used to estimate mercury exposure of piscivorous birds and sport fish when wildlife cannot be directly sampled.