A general computational alloy design approach based on thermodynamic and physical metallurgical principles, and coupled with a genetic optimization scheme, is presented. The method is applied to the design of new ultra-high-strength maraging stainless steels strengthened by Ni₃Ti intermetallics. In the first design round, the alloy composition is optimized on the basis of precipitate formation at a fixed ageing temperature without considering other steps in the heat treatment. In the second round, the alloy is redesigned, applying an integrated model which allows for the simultaneous optimization of alloy composition and the ageing temperature as well as the prior austenitization temperature. The experimental characterizations of prototype alloys clearly demonstrate that alloys designed by the proposed approach achieve the desired microstructures.