MoS₂ can be used as an excellent electrode material for lithium-ion batteries. However, the electrochemical performance of MoS₂ is not ideal due to its large volume changes during electrochemical processes, leading to its poor cyclic stability. Here, we report a simple and reliable hydrothermal carbonization method to prepare high-performance energy storage materials. Herein, using wheat straw as a carbon source and ammonium iron sulfate hexahydrate (AFSH) as a regulator, porous wheat straw carbon (PWSC) materials were prepared by hydrothermal and high-temperature carbonization treatment. Using the obtained porous carbon as a carbon matrix, a triblock copolymer F127 was selected to control the morphology of MoS₂, and a porous wheat straw carbon and flower-like MoS₂ composite (PWSC@MoS₂) was synthesized by hydrothermal method. The effects of the amount of structural modifier on the overall electrochemical properties of the composites were investigated. It was finally determined that the composite (PWSC@ MoS₂-2) at the optimal structural modifier ratio of 1:2 showed high lithium storage capacity (1435 mAh g⁻¹ after 100 cycles at 0.2 C), excellent cycling stability, and superior rate performance. Therefore, this efficient and environmentally friendly method of preparing PWSC@MoS₂ composites from wheat straw can realize the secondary utilization of biomass waste and is a new choice of anode materials for lithium-ion batteries.