A three-pass groove weld made by gas-tungsten arc welding in a 20-mm thick SA508 steel plate is modeled to predict the thermal, metallurgical, and mechanical behavior. The dilution for each pass is estimated as the proportion of base material in the weld metal, based on the predicted cross-sectional areas for the fusion zone (FZ) associated with each individual pass. The temperature predictions are consistent with the thermocouple measurement data and cross-weld macrographs. The predicted microstructures are qualitatively compared with the observed microstructures in cross-weld optical micrographs. The measured hardness is then used to quantitatively validate the predictions for postweld microconstituents (e.g., the ferrite, bainite, and martensite fractions), based on a hardness-microstructure correlation. The predicted residual stresses are compared with those measured by neutron diffraction. The results show that the dilution significantly affects the metallurgical and mechanical properties of weld metal (either as-deposited or reheated), and its consideration notably improves the predictions for microstructure and residual stress in the multipass steel weldment. Furthermore, the increase in dilution promotes the formation of martensite, which enhances the hardness, and leads to lower tensile stresses (or higher compressive stresses) in the weld metal. Such behavior arises due to the higher hardenability of the base material employed in this study, coupled with delayed austenite decomposition on cooling.