In this paper, single-crystalline Co7Fe3 nanowires were successfully electrodeposited into nanoporous anodic aluminum oxide (AAO) templates at different temperatures (20–60 °C). The morphology, crystallographic structure and magnetic properties of Co7Fe3 nanowires were studied. XRD and TEM results confirm that the Co7Fe3 nanowires have a <110> preferred orientation. With increasing bath temperature, the Co content is increased while Fe content is decreased in the Co7Fe3 nanowires. The compositional change in Co7Fe3 nanowires was investigated. Low bath temperature is beneficial to fabricate high-quality single-crystalline Co7Fe3 nanowires array and the growth mechanism of Co7Fe3 nanowires was also discussed. The hysteresis loop of the nanowires array demonstrates strong magnetic anisotropy with the easily magnetized direction being parallel to the nanowires axis. High coercivity (∼3440 Oe) and squareness (∼0.8) were obtained when the Co content is about 69 at.%. By controlling the growth conditions, we are able to prepare high-quality single-crystalline Co7Fe3 nanowires array with excellent magnetic properties.