Urea can be used as an effective hydrogen energy carrier, the development of efficient and stable anodic electrocatalysts for urea oxidation reaction (UOR) was crucial for achieved energy-saving hydrogen-production. Nanoflower like structures electrocatalysts have attracted increasing research interests due to its structural advantages. In this article, NiFeS/SSM with two dimensions (2D) nanosflower like structures in situ growth on three dimensions (3D) stainless steel mesh (SSM) is prepared by step-wise hydrothermal method. NiFeS/SSM was derived from NiFe layered double hydroxides, and the as-prepared electrode was directly served as a electrocatalysts for UOR. Benefiting from the electronic effect between Ni and Fe components which promotes the formation of the high valence Ni species in the NiFeS/SSM catalyst, the tuning effect from the in situ generated sulfate and its open 3D porous structure for SSM basement. The electrode displayed excellent catalytic activities towards UOR, the overpotential for UOR are 1.08 V in alkaline electrolyte at 50 mA·cm−2. This work not only illustrated that non-noble metal-based electrocatalysts have tremendous potential applications for electrocatalytic electrolysis of urea but also provided a feasible strategy to prepare high-efficiency and stable non-precious metal UOR anode catalysts in alkaline medium.