In this study, central composite circumscribed (CCC) design and response surface methodology (RSM) were used to model and optimize the electrodeposition characteristics of amorphous Fe-P alloys. Based on the results of a previous single-factor experiment, the significance of the influencing factors was determined using analysis of variance (ANOVA). Three factors significantly impacting the P content, hardness and corrosion current density of a deposit were identified: the bath temperature, pH and H2PO2− concentration. The statistical relationships between the process parameters and individual responses were established based on the CCC experimental data and RSM. The optimal parameters for each response were derived, and the influences of interaction terms were investigated. A desirability function was applied to determine the sample with the optimal comprehensive performance, featuring both high hardness and low corrosion current density. Due to the complex electrodeposition mechanisms of amorphous Fe-P alloys, the predicted P contents in deposits largely deviated from the experimental contents. However, the predictions of the hardness, corrosion current density and comprehensive performance were very accurate.