We report on the large-scale synthesis of Ag-nanoparticle (Ag-NP) decorated ZnO-mesoporous-nanosheets (NSs) grafted on a flexible carbon fiber cloth (CFC), as sensitive and reproducible surface enhanced Raman scattering (SERS) substrates with excellent flexibility. The composite SERS-substrates are achieved by a combination of atomic layer deposition of ZnO-seeds on each fiber of the CFC (denoted as ZnO-seeds@CFC), chemical bath deposition and subsequent pyrolysis for the creation of ZnO-mesoporous-NSs grafted on ZnO-seeds@CFC, and ion-sputtering of Ag-NPs on the ZnO-mesoporous-NSs. As abundant SERS "hot spots" are generated from the electromagnetic coupling of the densely distributed Ag-NPs, and the semiconducting ZnO-mesoporous-NSs also have chemical supporting enhancement and distinct molecule adsorbing abilities, the composite SERS-substrates demonstrate high SERS-sensitivity with good signal reproducibility. As a trial for potential applications, the composite SERS-substrates were used to identify pesticides and highly toxic polychlorinated biphenyls (PCBs), and low concentrations down to 10(-7) M for methyl parathion and 5 × 10(-6) M for PCB-77 were reached, respectively, showing promising potential for the SERS-based rapid detection of toxic organic pollutants in the environment.