To meet the future need for clean and sustainable energies, there has been considerable interest in the development of triboelectric nanogenerators (TENGs) that scavenge waste mechanical energies. The performance of a TENG at the macroscale is determined by the multifaceted role of surface and interface properties at the nanoscale, whose understanding is critical for the future development of TENGs. Therefore, various protocols from the atomic to the macrolevel for fabrication and tuning of surfaces and interfaces are required to obtain the desired TENG performance. These protocols branch out into three categories: chemical engineering, physical engineering, and structural engineering. Chemical engineering is an affordable and optimal strategy for introducing more surface polarities and higher work functions for the improvement of charge transfer. Physical engineering includes the utilization of surface morphology control, and interlayer interactions, which can enhance the active interfacial area and electron transfer capacity. Structural engineering at the macroscale, which includes device and electrode design/modifications has a considerable effect on the performance of TENGs. Future challenges and promising research directions related to the construction of next‐generation TENG devices, taking into consideration “interfaces” are also presented.