The weak interface and poor dispersion of carbon nanofillers in polymer matrix composites lead to a significant decrease in their performance, restricting the development of polymer nanocomposites. In this work, a highly facile strategy has been developed to improve the interfacial adhesion performance between graphene nanoplates (GNP) and thermoplastic polyurethanes (TPU) matrix via self‐polymerization of dopamine. Then, single‐walled carbon nanotubes (CNT), as reinforcing agent, were introduced into surface modified GNP solution to prepare the corresponding ternary composites. Scanning electron microscope images show that GNP and CNT formed 3‐D interconnecting network‐like architecture. The sample modified with three layers of nonwoven fabric decorated with 1.0 mg/mL nanomaterial exhibit a tensile strength 35% higher than that of the virgin TPU. Consequently, compared with virgin TPU, the erosion resistance and thermal conductivity are enhanced by 78% and 45%, respectively.