In targeting the most important energy and environmental issues in current society, the development of low-cost, bifunctional electrocatalysts for urea-assisted electrocatalytic hydrogen (H-2) production is an urgent and challenging task. In this work, interlaced rosette-like MoS2/Ni3S2/NiFe-layered double hydroxide/nickel foam (LDH/NF) is successfully synthesized by a two-step hydrothermal reaction. Due to its unique interlaced heterostructure, MoS2/Ni3S2/NiFe-LDH/NF exhibits excellent bifunctional catalytic activity towards the urea oxidation reaction (UOR) and the hydrogen evolution reaction (HER) in 1.0 M KOH with 0.5 M urea. In a concurrent two-electrode electrolyser (MoS2/Ni3S2/NiFe-LDH/NF(+,-)), only voltage of 1.343 V is required to reach 50 mA cm(-2), which is 216 mV lower than for pure water splitting. Furthermore, after 16 h of urea electrolysis in 1.0 M KOH with 0.5 M urea, the current density remains at 98% of the original value. Thus, the catalyst is not only favorable for H-2 production, but also has great significance for the problem of urea-rich wastewater treatment. (C) 2019 Hydrogen Energy Publications LLC. Published by Elsevier Ltd. All rights reserved.