In this paper, dandelion-like ZnS was synthesized via a facile hydrothermal method, and then as the support to further synthesize dandelion-like ZnS/carbon quantum dot hybrid materials. Multiple techniques were applied to investigate the structures, morphologies, electronic and optical properties of the samples. It can be observed that the carbon quantum dots were distributed uniformly on the surface of the ZnS. The photocatalytic activities of the as-prepared materials were investigated by the photodegradation of methylene blue, Rhodamine B and the colorless antibiotic ciprofloxacin hydrochloride, respectively. The as-synthesized hybrid materials exhibit higher photocatalytic activity than that of the pure ZnS under simulated sunlight (λ > 380 nm), indicating a broad-spectrum of photocatalytic degradation activity. The most beneficial amount of carbon quantum dots to improve the photocatalytic activity of the ZnS is 2.0 wt%.