Search for appropriate materials with favorable staggered energy band arrangements is important and of great challenge to fabricate Z-scheme photocatalysts with high activity in visible light. In this study, we demonstrated a facile and feasible strategy to construct highly active organic-inorganic Z-scheme hybrids (P-BMO) with linear pyrene-based conjugated polymer (P17-E) and Bi2MoO6 via in-situ palladium-catalyzed cross-coupling reaction. Characterization results revealed C-O chemical bond formed at the heterointerface between P17-E and Bi2MoO6 after in-situ polycondensation and endowed the hybrids with observably improved photogenerated carries transfer capability. Visible light driven photocatalytic removal of ciprofloxacin and Cr(VI) were significantly enhanced after the incorporation of P17-E into Bi2MoO6 whether with the morphology of nanosheets, nanobelts or microspheres. Moreover, this P-BMO hybrids were also found to exhibit sustainable excellent photocatalytic performance after four runs of photocatalytic evaluation test, suggesting its high activity and stability. To better eliminate the redox ability enhancement of P-BMO, a reasonable Z-scheme electrons transferring mechanism between P17-E and Bi2MoO6 was proposed and proved by the determination of •O2– and •OH and Pt nanoparticles photodeposition experiments. This work might provide a viable source and insight into the design of Z-scheme photocatalysts with excellent redox ability for environmental remediation.