Urea degradation is a viable method to produce hydrogen in a sustainable way, while having an important place in environmental protection and energy security. In this work, ultrathin N-doped carbon (NC) nanosheets, modified by ultrafine multiple transition metal sulfide (NiFeCoZn–S) nanoparticles, are synthesized to serve as electrocatalysts for overall urea degradation. This unique structure allows NiFeCoZn–S/NC to have a relatively large ECSA and active sites, stemming from the small dimensions of the NiFeCoZn–S particles and the hierarchical nanoarchitecture of the NC. Thus, NiFeCoZn–S/NC has a significant urea oxidation reaction (UOR) activity of 1.31 V at 10 mA cm−2 in an electrolyte consisting of 1.0 M KOH and 0.33 M urea. Furthermore, when the catalyst was used in an electrolytic cell for urea degradation, a potential of 1.49 V was achieved up to 10 mA cm−2. Additionally, the catalyst exhibits only a 6.1 % performance decay after 660 h of operation at 10 mA cm−2. Its exceptional stability outshines that of existing urea catalysts, rendering it an attractive prospect for future applications.