To fabricate a novel photocatalyst material with high efficiency, ZnO seeds were uniformly deposited on carbon fibers (CFs) via atomic layer deposition (ALD) followed by hydrothermal growth of ZnO nanorods (NRs). Then Pt particles were dispersed on ZnO NRs using the magnetron sputtering method, and the grain size of Pt particles was in the range of 2–5 nm. Significantly, the resultant Pt@ZnO NRs/CFs composites exhibited better photocatalytic performance than normal ZnO NR coated CFs as demonstrated in the degradation of methyl orange (MO) solution, which may be due to the synergistic effect between the Pt nanoparticles and ZnO NRs. After a period of light irradiation, the degradation rates of methyl orange (MO) dye solution are as follows: 72% for ZnO NRs/CFs and 99.8% for Pt@ZnO NRs/CFs. In addition, this novel hierarchical photocatalyst can be easily recycled with good performance and stability.