A novel catalytic material of MOF-based In2S3-X2S3 (X = Bi; Sb)@TFPT-COFs hybrids was designed and synthesized by using an interface ion-exchange method with MOFs as the precursors. The hybrid materials were fabricated by combining heterojunctions with TFPT-COFs through C=N bonds. The functionalization of the amino groups on the heterojunction surface was a crucial step to construct the MOFs@COFs hybrid materials. The resulting samples were hierarchical tubular nanostructures with uniform nano-scale interfacial contacts. The doping of Bi3+ or Sb3+ further facilitated the construction of heterojunctions to reduce the band gap value of In2S3 and extended light absorption range. The synergistic effect between the frameworks contained in In2S3-X2S3 (X = Bi; Sb) and the triazine frameworks of TFPT-COFs was conducive to accelerating charge transportation and separation. The photo-erosion of heterojunctions could also be prevented by the encapsulated TFPT-COFs sheets. Noteworthily, the photocatalytic degradation abilities of hexavalent chromium, ponceau-4R and rhodamine B were significantly improved after the introduction of TFPT-COFs . Especially, In2S3-X2S3@TFPT-COFs performed excellent photocatalytic reduction activity. Approximately 100% of aqueous Cr(VI) was photo-reduced within only 5 min. Based on the experimental results of UV-Vis adsorption spectra and ESR spectra, a possible mechanism was proposed to explain the excellent photocatalytic performance of the photocatalytic system.