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Funding Information: We acknowledge support from the European Union Horizon 2020 research and innovation program under NOMATEN Teaming grant (agreement no. 857470) and from the European Regional Development Fund via the Foundation for Polish Science International Research Agenda PLUS program grant No. MAB PLUS/2018/8. We acknowledge the computational resources provided by the High Performance Cluster at the National Centre for Nuclear Research in Poland. Y.Z. H.B. and W.J.W. were supported as part of the Energy Dissipation to Defect Evolution (EDDE), an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Basic Energy Sciences under contract number DE-AC05-00OR22725. ; Significant hardening effect due to Fe concentrations in Ni-based alloys with face-centered-cubic structure has been studied by using a combined experimental and atomistic-based computational approach via nanoindentation tests. The obtained experimental load–displacement data for the [0 0 1] crystal orientation reached a qualitative good agreement with molecular dynamics simulations results, leading to strong evidence that the main strengthening factors are associated to sluggish dislocation diffusion, reduced defect sizes and the nucleation of tetrahedral stacking faults. Here, interstitial type prismatic dislocation loops mainly formed by ⅙〈1 1 2〉 Shockley dislocations are nucleated during the loading process, where their interaction leads to the formation of pyramidal shaped stacking fault which are mainly created by ⅓〈1 0 0〉 Hirth dislocations lines. Observing both types of defects coexisting in the same plastic deformation zone by both approaches. Reported mechanical data, measured experimentally and interpreted numerically, are also in accordance with microstructural SEM and TEM investigations. ; Peer reviewed