Design of accident tolerant fuel (ATF) cladding materials demands large amounts of time and experimental efforts with the conventional trial-and-error method. In this work, the ab initio coupled CALPHAD (CALculation of PHAse Diagrams) approach has been performed on FeCrAl based and MAX-phase related systems. Phase diagrams have been constructed to reproduce and rationalize the literature data. Key experiments were also carried out to validate the present calculations. Meanwhile, the thermochemical, physical and elastic mechanical properties are well described. This correlative research strategy may enhance the efficiency in designing new ATF cladding materials by promoting the discovery of the composition-structure-property-performance relationships.