The signal crosstalk and electromagnetic interference (EMI) problems direly need to be resolved in the rapid development of modern microwave communication technology for a better working frequency and transmission power of electronic systems. Where the new absorbing materials such as molybdenum disulfide (MoS₂)/titania (TiO₂)/Ti₂CT_x and MoS₂/Ti₂CT_x composites could meet the requirement of “thin, strong, light weight, and wide band” for excellent absorbing performance. In this work, a lighter Ti₂CT_x material was selected as the matrix, and MoS₂ was in-situ grown on Ti₂CT_x matrix by traditional hydrothermal method and microwave solvothermal method. The fabricated composite exhibited synergic effect of two-dimensional heterostructural interface and double dielectric elements, where the small amount of TiO₂ and the certain proportion of TiO₂(Ti₂CT_x oxide) with MoS₂ improve the impedance matching to -54.70 dB RL_min and EAB_max of 4 GHz. Polyethylene glycol 200 was used as the solvent instead of water to make Ti₂CT_x less oxidized during the composite process, where the microwave heating would attain fast speed, short time, high efficiency, and uniform product. Since, the MoS₂/Ti₂CT_x composite without oxidizing possessed a wider EAB at a thinner thickness, thus resulting in the excellent microwave absorption performance and confirming the validity and rationality of new microwave absorption materials.