The modification of ZnO, such as transforming it from 1‐D to 3‐D nanostructures or compositing it with carbon‐based materials, has been extensively explored to enhance light energy harvesting and reduce electron‐hole recombination‐key limitations of ZnO. Herein, the effect of different composite materials, specifically nitrogen‐doped carbon quantum dots (N‐CQDs) and nitrogen, sulfur‐doped carbon quantum dots (N,S‐CQDs), on ZnO's morphology and photocurrent response was studied. Various morphologies were synthesized on conductive glass substrate using a one‐pot hydrothermal method, including flower‐like structure for ZnO/N‐CQDs (∼d = 0.9 µm) and multilayered microspheres for ZnO/N,S‐CQDs (∼d = 1.1 µm). The inclusion of sulfur atoms in the composite resulted in a reduced bandgap value from 3.22 to 3.11 eV, along with enhanced light absorption efficiency and improved separation of photogenerated electron‐hole pairs. Furthermore, the crystallinity of ZnO/N,S‐CQDs was significantly enhanced compared to ZnO without sulfur doping. These improvements were reflected in the photoelectrochemical (PEC) measurements, where ZnO/N,S‐CQDs showed a current density of 21.8 µA/cm2 at 0.5 V (vs. Ag/AgCl), which is 5.5 times higher than that of ZnO/N‐CQDs (4.0 µA/cm2). These findings demonstrate that sulfur doping improves photocatalytic efficiency, making 3D ZnO/N,S‐CQDs a promising candidate for various UV‐driven PEC applications.