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Abstract Thermal interfaces are vital for effective thermal management in modern electronics, especially in the emerging fields of flexible electronics and soft robotics that impose requirements for interface materials to be soft and flexible in addition to having high thermal performance. Here, a novel sandwich‐structured thermal interface material (TIM) is developed that simultaneously possesses record‐low thermal resistance and high flexibility. Frequency‐domain thermoreflectance (FDTR) is employed to investigate the overall thermal performance of the sandwich structure. As the core of this sandwich, a vertically aligned copper nanowire (CuNW) array preserves its high intrinsic thermal conductivity, which is further enhanced by 60% via a thick 3D graphene (3DG) coating. The thin copper layers on the top and bottom play the critical roles in protecting the nanowires during device assembly. Through the bottom‐up fabrication process, excellent contacts between the graphene‐coated CuNWs and the top/bottom layer are realized, leading to minimal interfacial resistance. In total, the thermal resistance of the sandwich is determined as low as ~0.23 mm² K W⁻¹. This work investigates a new generation of flexible thermal interface materials with an ultralow thermal resistance, which therefore renders the great promise for advanced thermal management in a wide variety of electronics.