Thermal interface materials (TIMs) play a crucial role in enhancing the reliability and sustainable utilization of next-generation electronics and thus can help meet the increasing demand for multifunctional devices with higher performance. Herein, we introduce a method for creating a TIM with high cross-plane thermal conductivity based on graphite nanoplatelet (GNP)/polyurethane (PU) films. The graphite nanoplatelets ensured the heat transfer properties of the TIM. Moreover, the hot-pressing procedure improved the thermal conductivity to 26.3 W (m K)−1 with the improved orientation of the GNPs in the PU matrix, as confirmed by microscopy investigation. Under a thermal dissipation power of 10–20 W, a drastic reduction in the chip temperature (17.5–42.3 °C) was achieved using our oriented GNP/PU TIM compared to a commercial silicone TIM (5.0 W (m K)−1). In addition, as-prepared pads can be mass produced at an acceptable cost, indicating that our work provides a promising new approach to fabricating TIMs for application in the next-generation thermal management of high power density electronics.