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[Display omitted] • Metal polymeric composites based on pyrimidine-functionalized COFs (covalent organic frameworks) were fabricated. • Fe@COF-Pyr composite possesses good catalytic performance for oxygen evolution reaction. • Au-Pd@COF-Pyr can promote methane oxidation. Functionalized covalent organic frameworks (COFs) materials are used in various fields due to their unique properties. Herein, the reported pyrimidine-functionalized COFs sample named COF-Pyr is selected as the matrix to provide two COFs-based metal composites Fe@COF-Pyr and Au-Pd@COF-Pyr, which are respectively synthesized through metal coordination and in situ reduction reaction. On the one hand, Fe@COF-Pyr used as the electrocatalyst exhibits a good oxygen evolution reaction activity with the overpotential of only 430 mV at a current density of 10 mA cm−2 in the KOH solution (1 M) electrolyte. It is attributed to the large specific surface area (427 m2/g) and abundant catalytic sites of Fe@COF-Pyr, which help to improve the electrochemical performance. On the other hand, Au-Pd@COF-Pyr is an excellent catalyst for methane conversion that the products of the methane oxidation reaction can be obtained under mild reaction conditions. This work not only provides a newfangled notion for the design and preparation of COFs-based metal composites but also broadens the practical application of COFs materials in the domain of catalysis. [ABSTRACT FROM AUTHOR]