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. Plasma‐enhanced chemical vapor deposition of copper films is achieved in ambient air and at low temperature using a helium dielectric barrier discharge jet. The deposited copper films are characterized. Film deposition is also achievable on temperature‐sensitive substrates, such as plastic, cardboard, agar, and pork skin.