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While high-aspect-ratio metal nanowires are essential for producing nanowire-based electrodes of good performance used in electronics and electrocatalysis, the synthesis of millimeter-long Cu nanowires remains a challenge. This work demonstrates an oleylamine-mediated hydrothermal method for synthesis of Cu nanowires with an average diameter of ~80 nm and a length up to several millimeters. An investigation on the role of oleylamine in nanowire formation by mass spectroscopy, small angle X-ray diffraction and transmission electron microscopy reveals that oleylamine serves as a mild reducing agent for slow reduction of Cu(II) to Cu, a complexing agent to form Cu(II)-oleylamine complex for guiding the nanowire growth, as well as a surfactant to generate lamellar phase structure for the formation of nanowire bundles. The growth mechanism of these millimeter-long Cu nanowire bundles is proposed based on the experimental observations. Electrochemical measurements by linear sweep voltammetry indicate that the self-supported nanowire electrode prepared from as-formed Cu nanowire bundles shows high catalytic activity for electroreduction of nitrate in water.