The three-dimensional porous Fe3O4@Cu2-xS-MoS2 framework is reported for the first time. The as-prepared 3D framework exhibits good structural stability, high surface area, enhanced adsorption capacity to substrates, and strong absorption in the NIR range. As a result, such hybrid frameworks exhibit excellent NIR-light photocatalytic activity and stable cycling for the direct arylation of heteroaromatics at room temperature.