Nitrogen-doped carbon nanotube confined CuCo nanoalloy catalysts are fabricated by using ZIF-67 as a sacrificial template for the one-pot selective hydrogenation of levulinic acid (LA) to 1,4-pentanediol (1,4-PDO). The optimal catalyst achieves a high 1,4-PDO yield of 87.8% at full LA conversion. It also exhibits good recycling stability and can be reused at least 5 times.