In this paper, we report a simple and reliable hydrothermal synthesis strategy to prepare high-performance energy storage materials. Herein, polyvinylpyrrolidone (PVP) was added to obtain spherical MoS2 composite wheat straw cellulose carbon material (MoS2 @WSCC-S), and ammonium persulfate (APS) was further added under acidic conditions to obtain 3D nanoflower-like MoS2 grown on wheat straw cellulose carbon (MoS2 @WSCC-F). These results unequivocally demonstrate that the presence of oxygen-containing groups and the pH of the solution are key factors enabling the formation of flower-like structures, with MoS2 uniformly decorated on the wheat straw cellulose carbon. Mo at the edge of MoS2, C in PVP molecules, and oxygen-containing functional groups released by APS are directly coupled with wheat straw cellulose carbon (C-O-Mo bond). The interfacial interaction of the C-O-Mo bond can enhance the electron transport rate and structural stability of the MoS2 @WSCC-F electrode. The wheat straw cellulose carbon enhances the electrical conductivity of the composite and maintain structural integrity, and at the same time, it can not only serve as a substrate for uniformly dispersing active MoS2, but also serve as a buffer to accommodate volume changes during cycling. As a negative electrode material for lithium-ion batteries, the obtained MoS2 @WSCC-F has a stable charge-discharge capacity of 1056.3 mAh g−1 after 300 cycles at a 1 C rate, a first-cycle Coulombic efficiency of 77 %, and a capacity retention rate of 80.4 %.