MoS2 has been extensively investigated as anode material in lithium-ion batteries (LIBs). However, the poor stability of MoS2 due to the weak interaction with conductive support and current collector significantly hinders its performance in LIBs. In this work, the Ni3S2 interlayer was successfully in-situ formed between MoS2 and Ni foam by decomposing MoS2 precurors ((NH4)2MoS4) on Ni foam (denoted as MoS2/Ni3S2/Ni). The presence of Ni3S2 interlayer significantly enhanced the interaction between MoS2 and Ni foam support, resulting in excellent stability in lithium-ion batteries. In addition, the foam structure facilitates the ion diffusion and electron transport properties of the electrode materials, leading to high-rate and highly durable performance. The as-prepared MoS2/Ni3S2/Ni reveals a capacity of 1263mAhg−1 after 100 cycles at a current density of 0.1Ag−1. On the other hand, it shows excellent rate performance, and it’s capacity can maintain at 740mAhg−1 even at a high current density of 10Ag−1. The interlayer strategy provides a novel principle for the design of durable electrode materials in electrochemical energy storage devices. In this work, for the first time, the Ni3S2 interlayer was successfully in-situ formed between MoS2 and Ni foam by decomposing MoS2 precursors ((NH4)2MoS4) on Ni foam resulting in excellent performance in lithium-ion batteries. The interlayer strategy provides a novel principle for the design of electrode materials in electrochemical energy storage devices.