Cyanobacterial harmful algal blooms and the toxins they produce are a global water-quality problem. Monitoring and prediction tools are needed to quickly predict cyanotoxin action-level exceedances in recreational and drinking waters used by the public. To address this need, data were collected at eight locations in Ohio, USA, to identify factors significantly related to observed concentrations of microcystins (a freshwater cyanotoxin) that could be used in two types of site-specific regression models. Real-time models include easily- or continuously-measured factors that do not require that a sample be collected; comprehensive models use a combination of discrete sample-based measurements and real-time factors. The study sites included two recreational sites and six water treatment plant sites. Real-time models commonly included variables such as phycocyanin, pH, specific conductance, and streamflow or gage height. Many real-time factors were averages over time periods antecedent to the time the microcystin sample was collected, including water-quality data compiled from continuous monitors. Comprehensive models were useful at some sites with lagged variables for cyanobacterial toxin genes, dissolved nutrients, and (or) nitrogen to phosphorus ratios. Because models can be used for management decisions, important measures of model performance were sensitivity, specificity, and accuracy of estimates above or below the microcystin concentration threshold standard or action level. Sensitivity is how well the predictive tool correctly predicts exceedance of a threshold, an important measure for water-resource managers. Sensitivities >90% at four Lake Erie water treatment plants indicated that models with continuous monitor data were especially promising. The planned next steps are to collect more data to build larger site-specific datasets and validate models before they can be used for management decisions.