Abstract1-aminoperylene diimide/TiO2/MoS2 composite (NH2-PDI/TiO2/MoS2) with ordered structure was prepared by hydrothermal synthesis method. The composite was characterized by XRD, SEM, FTIR, XPS, BET, DRS, PL, EIS, Raman, photocurrent, and Mott-Schottky plots spectroscopy. The potential positions of the conduction and valence bands, and the band gap energy of the semiconductors were estimated. The composite exhibited higher photocatalytic activity compared with the mono-component systems. The apparent rate constants (k) were determined as 0.00616, 0.00352, 0.00738, 0.00517, 0.00752, and 0.00806 min−1 for TiO2, NH2-PDI, NH2-PDI/TiO2, MoS2, MoS2/TiO2, and NH2-PDI/TiO2/MoS2, respectively. The detection of radical scavengers confirmed that superoxide radicals, photogenerated holes, and photogenerated electrons were the main active substances for MB degradation. Between type II- heterojunction mechanism and Z-scheme mechanism, the latter could explain the enhanced photocatalytic activity of the composite better. The Z-scheme mechanism accumulates more electrons at CB level of NH2-PDI and hence generates more super oxide radicals.