The development of metal-free heterogeneous catalysts for advanced oxidation processes has emerged as a key focus for both academia and industry. We report on research that seeks to establish a correlation between the crystallographic, physicochemical, textural, and morphological properties of a series of graphite-based solids and their activities as metal-free ozonation catalysts in aqueous media. Our findings show that nanographite (NG) outperforms traditional graphite-based solids, activated carbon and Co3O4. The enhanced activity of NG is due to defective nanosized graphitic structures with high surface areas. NG exhibits an exceptional activity, durability, and recyclability that surpasses other known catalysts. Our study employs electron spin resonance and selective quenching experiments that reveal the generation of 1O2 during catalytic ozonation. Significantly, NG shows excellent catalytic efficiency even when using natural surface river water or seawater. This study illustrates the importance of the natural properties of graphite-based materials as active and durable ozonation catalysts in water.