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The present article deals with effect of Cr addition (10 at.%) on the partitioning behavior and the consequent effect on mechanical properties for tungsten-free γ-γ′ cobalt-based superalloys with base alloy compositions of Co-30Ni-10Al-5Mo-2Ta (2Ta) and Co-30Ni-10Al-5Mo-2Ta-2Ti (2Ta2Ti). Cr addition leads to a change in the morphology of the strengthening cuboidal-shaped γ′ precipitates to a spherical shape. The site preference of Cr atoms in two alloy systems (with and without Ti) has been experimentally investigated using atom probe tomography with the supportive prediction from first principles DFT-based computations. Cr partitions more to the γ matrix relative to γ′. However, Cr also has a strong effect on the Ta and Mo partitioning coefficient across γ/γ′ interfaces. The value of partition coefficient for Mo ( K ) becomes <1 with Cr addition to the alloys. Results from ab initio calculations show that the Cr atoms prefer to replace Mo atoms in the sublattice sites of the L1 unit cell. The solvus temperature of about 1038 and 1078 °C was measured for 10Cr2Ta and 10Cr2Ta2Ti alloy, respectively, and these Cr-containing alloys have very low densities in the range of ~8.4-8.5 gm/cm. The 0.2% compressive proof strength of 10Cr2Ta2Ti alloy yields a value of 720 MPa at 870 °C, substantially better than most Co-Al-W-based alloys and many of the nickel-based superalloys (e.g., MAR-M-247). [ABSTRACT FROM AUTHOR]