Anthropogenic release of polycyclic aromatic hydrocarbons (PAHs) in water bodies has raised global concerns due to their notorious toxicity and carcinogenicity, therating aquatic exosystems and human well-being. Adsorption processes have been proposed for PAHs remediation, but their practical applications are limited by the lack of high-performance adsorbents and effective manufacturing processes. Here, we present a facile and scalable method to produce a COF-300/PVDF composite as a high-performance adsorbent for PAHs removal. The composite comprises a porous PVDF substrate containing numerous aligned microchannels in its entire cross-section where COF-300 is fully coated. The adsorption capacities of the COF-300 powder towards two sample PAH pollutants, i.e. naphthalene and 1-naphthylamine, are 655 and 570 mg g−1, respectively, which are among the highest reported values. The composite adsorbent demonstrates better adsorption kinetics and removal efficiencies than the COF-300 powders at the same feed input of 1.44 L h-1g−1, and its superior performance has been further highlighted through a comparative study with a COF-300 pack column and COF-300/PVDF mixed matrix membranes. These results suggest that the newly developed COF-300/PVDF composite holds great potential in practical applications for PAHs removal.