Nanostructuring of electrocatalysts is an important aspect of catalyst design as catalytic performance depends not only on the specific activity (reaction rate per surface area), but also on the dispersion of the catalyst. We present an industrially compatible, but effective preparation method for support-free nanostructured catalyst layers. Alternating sputtering was used to prepare heterogeneous Pt–Cu templates ranging from 95 up to 99.5 at. % Cu. These templates were then electrochemically leached to form a nanostructured Pt–Cu network and benchmarked with respect to the oxygen reduction reaction. It is shown that the templates with lower Cu:Pt ratios exhibit the highest initial specific activity but have a relatively low electrochemically active surface area. Subjecting the samples to extended accelerated stress tests, it is found that the support-free nanostructured Pt–Cu networks are relatively resistant to high potential cycling, which can be explained by the lack of carbon corrosion. The loss in electrochemical surface area thereby depends on the initial Pt content. The specific oxygen reduction activity, however, approaches the value of bulk Pt. Although this decrease is not desirable, still an (specific) activity improvement of two to four times as compared carbon supported nanoparticles can be preserved.