Lithium metal anode (LMA) possesses the largest energy density among all anode candidates, while dendrite growth is a huge barrier in the direct application of LMA in batteries. Herein, metal–organic framework (MOF) derived Zn–CxNy nanoparticle arrays are newly grown onto carbon cloth as an effective host toward lithium metal anode. The N and Zn species are lithiophilic to Li-ions, resulting in a stable Li plating/stripping process of up to 2300 h without running into a dendrite issue when operating at a current density of 10 mA cm−2. The newly developed ZNCC-Li anode also exhibits an ultralow voltage hysteresis of only 6.4 mV at the end of the operating process. This work creates an effective design of MOF-derived lithium metal anode suitable for high-energy batteries.