With the macroscale and conductive carbon fiber cloth (CFC) as the substrate, the obtained self-supported photocatalysts hold great promise for enhancing the separation of generated carriers and the recyclability of catalysts, thereby improving the photocatalytic performance and practicality in various applications. Additionally, decorating metal-organic frameworks (MOFs) with ultrahigh surface area on the surface of effective semiconductors is a promising method to enhance the adsorption capacity and photocatalytic performance. Herein, zeolitic imidazolate framework-67 (ZIF-67) as a typical MOFs was applied to modify carbon nitride (C 3 N 4 ) on the surface of macroscale and conductive CFC. CFC/C 3 N 4 /ZIF-67 (4 × 4 cm 2 ) was obtained by a thermal condensation-chemical bath deposition two-step route, and it shows superior adsorption and photocatalytic activity toward bisphenol A (BPA), levofloxacin (LVFX), ciprofloxacin (CIP) and good hydrogen evolution activity. Besides, the recycling test for four cycles indicates the high stability of CFC/C 3 N 4 /ZIF-67 with an easy recycling process. In this study, CFC/C 3 N 4 /ZIF-67 was prepared through the hydrothermal and chemical bath deposition two-step method, which enhances light absorption and photocatalytic performance, as well as recyclability for solving environmental and energy issues.