A highly effective oxidation cross-coupling method involving p-cresol derivatives and malonitrile derivatives has been developed utilizing undivided electrolytic conditions. This electrochemical approach offers a robust route to synthesizing diverse malonitrile derivatives featuring quaternary carbon centers incorporating para-phenol groups. Notably, the direct electro-oxidation of the C(sp3)-H bond in the p-cresol derivative plays a crucial role in this process under electrolytic conditions. Various p-cresol derivatives and malonitrile derivatives with different substituents are readily compatible with this electrochemical transformation, affording coupling compounds with up to 99% yield.