In this work, half the mass of carbon black (CB) was replaced by lignin for preparation of high-performance nitrile rubber/poly(vinyl chloride) composites via constructing interfacial Zn2+-based coordination bonds. It was demonstrated that lignin played a significant role as a natural ligand to form the Zn2+-based coordination interactions in the interphase between lignin and a rubber matrix. The tensile strength and Young's modulus of the composites were significantly enhanced by the Zn2+-based coordination bonds owing to the dynamic fracture of coordination bonds. The thermo-oxidative aging resistance of the composites was improved by lignin and could be conveniently regulated by the content of ZnCl2 and sulfur. The high-temperature oil resistance of the composites also benefited from the partial substitution of CB by lignin and incorporation of the metal coordination bonds. This work opens a facile method for the potential application of green lignin in rubber-plastic composites through a conventional rubber compounding process.