Two novel techniques are combined for the design of novel alloys for enhanced strength/ductility relationships: (1) a principal component analysis on an extensive database of commercial alloys; and (2) thermostatistical modelling of alloy plasticity, which allows to capture the overall stress-strain curve as a function of composition and microstructure. The combined models are validated with hundreds of Fe-base alloys, and it is demonstrated that strength/ductility improvements are still possible by altering both microstructre and composition. By combining the models with a third approach, an artificial neural network, new alloys exhibiting strength/ductility relationships beyond existing technology are conceived. This fits within the Accelerated Metallurgy programme, a major European effort towards the discovery of novel alloys to satisfy modern industrial and environmental needs.