The deformation behavior of nanoporous metal (NPM) is important for their wide range of applications. Strain hardening can effectively enhance the resistance to the deformation. Here we report a novel nanoporous CrFe alloy with ordered structure, which is fabricated by selective phase dissolution of the two-phase Al–Ni–Fe–Cr high entropy alloy. The formation mechanism, microstructure and deformation behavior are investigated in details. The ordered nanoporous CrFe alloy behaves rapid strain hardening and high resistance to deformation. The regular skeletons can be entirely compacted between parallel two sides, which facilitates the densification of nanoporous alloy. Lots of internal boundaries are generated and act as barriers for the dislocation motion. This would favor of the improvement of strain hardening.