AbstractVoltage‐driven manipulation of magnetism in electrodeposited 200 nm thick nanoporous single‐phase solid solution Cu₂₀Ni₈₀ (at%) alloy films (with sub 10 nm pore size) is accomplished by controlled reduction‐oxidation (i.e., redox) processes in a protic solvent, namely 1 m NaOH aqueous solution. Owing to the selectivity of the electrochemical processes, the oxidation of the CuNi film mainly occurs on the Cu counterpart of the solid solution, resulting in a Ni‐enriched alloy. As a consequence, the magnetic moment at saturation significantly increases (up to 33% enhancement with respect to the as‐prepared sample), while only slight changes in coercivity are observed. Conversely, the reduction process brings Cu back to its metallic state and, remarkably, it becomes alloyed to Ni again. The reported phenomenon is fully reversible, thus allowing for the precise adjustment of the magnetic properties of this system through the sign and amplitude of the applied voltage.