This study investigates the use of covalent organic frameworks (COFs) as photocatalysts to tackle water pollution. COFs, known for their adjustable porosity, robust stability, and selective adsorption, are particularly effective in removing contaminants from water, showing significant promise for applications of environmental science. The experiment applied atmospheric-pressure microplasma to synthesize COFs—a green chemistry technique that enables synthesis at room temperature using water as a solvent, avoiding the need for high temperatures or harmful chemicals, and completing the process within one hour. Our results showed that the synthesized COFs can effectively degrade common dye pollutants, such as crystal violet and methylene blue, exhibiting high photocatalytic efficiency. UV-visible spectroscopy data revealed that the main absorbance peaks of these dyes diminish and nearly vanish as the photocatalytic reaction proceeds, affirming the COFs’ strong degradation abilities. The images from scanning electron microscopy highlight the COFs’ ordered porous structure, which contributes to their catalytic effectiveness and stability. In conclusion, our proposed approach not only provides a powerful solution for treating organic pollutants in water but also presents vast potential for environmental protection and water pollution control on a global scale.