The classic Cantor (FeCoCrMnNi) isoatomic high entropy alloy was modified by separate additions of Mo and Nb in an effort to optimize its mechanical properties and sliding wear response. It was found that the introduction of Mo and Nb modified the single phase FCC solid solution structure of the original alloy and led to the formation of new phases such as the BCC solid solution, σ-phase, and Laves, along with the possible existence of intermetallic phases. The overall phase formation sequence was approached by parametric model assessment and solidification considerations. Nanoindentation-based mechanical property evaluation showed that due to the introduction of Mo and Nb; the modulus of elasticity and microhardness were increased. Creep nanoindentation assessment revealed the beneficial action of Mo and Nb in increasing the creep resistance based on the stress sensitivity exponent, strain rate sensitivity, and critical volume for the dislocation nucleation considerations. The power law and power law breakdown were identified as the main creep deformation mechanisms. Finally, the sliding wear response was increased by the addition of Mo and Nb with this behavior obeying Archard’s law. A correlation between microstructure, wear track morphologies, and debris characteristics was also attempted.