This study demonstrates that plasma‐enhanced chemical vapor deposition of copper films can be achieved in ambient air and at low temperature. A helium dielectric barrier discharge jet with a small mixture of hydrogen and copper(II) acetylacetonate vapor is utilized as the nonthermal plasma source to deposit conductive copper films with low electrical resistivity (<1 × 10−7 Ω·m). The deposited film appears to have three distinct regions (reddish brown, dark blue, and yellowish) from center to edge. Copper nanograins (~50 nm) are observed in both the reddish‐brown and the dark‐blue regions, whereas the yellowish region exhibits a continuous structure containing copper oxide. The copper films are further deposited on various temperature‐sensitive substrates, including plastic, cardboard, agar, and pork skin. [ABSTRACT FROM AUTHOR]