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Doping with Co and Fe is a promising strategy to enhance the performance of Ni‐Mn‐based magnetocaloric materials. We investigate here the impact of these two elements on the magnetic properties and the martensitic transformations in Mn‐rich Ni‐Mn‐Al Heusler alloy. Based on ab initio ground‐state energies, we explain the martensitic transformation temperatures in these alloys. The magnetic ground states of the austenite and the martensite phases are discussed on the basis of magnetic exchange parameters. A thorough comparison of the transition temperatures and the change in saturation moments during martensitic transformation brings into light the relative potential of the two substitutional elements for future applications.