Metallic nanofoams, cellular structures consisting of interlinked thin nanowires and empty pores, create low density, high surface area materials. These structures can suffer from macroscopically brittle behavior. In this work, we present a multiscale approach to study and explain the mechanical behavior of metallic nanofoams obtained by an electrospinning method. In this multiscale approach, atomistic simulations were first used to obtain the yield surfaces of different metallic nanofoam cell structures. Then, a continuum plasticity model using finite elements was used to predict the alloy nanofoam's overall strength in compression. The manufactured metallic nanofoams were produced by electrospinning a polymeric non-woven fabric containing metal precursors for alloys of copper–nickel and then thermally processing the fabric to create alloy metallic nanofoams. The nanofoams were tested with nanoindentation. The experimental results suggest that the addition of nickel increases the hardening of the nanofoams. The multiscale simulation modeling results agreed qualitatively with the experiments by suggesting that the addition of the alloying can be beneficial to the hardening behavior of the metallic nanofoams and helps to isolate the effects of alloying from morphological changes in the foam. This behavior was related to the addition of solute atoms that prevent the free dislocation movement and increase the strength of the structure.