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Techniques for scaling-up the direct-current (dc) triboelectricity generation in MoS2multilayer-based Schottky nanocontacts are vital for exploiting the nanoscale phenomenon for real-world applications of energy harvesting and sensing. Here, we show that scaling-up the dc output can be realized by using various MoS2multilayer-based heterojunctions including metal/semiconductor (MS), metal/insulator (tens of nanometers)/semiconductor (MIS), and semiconductor/insulator (a few nanometers)/semiconductor (SIS) moving structures. It is shown that the tribo-excited energetic charge carriers can overcome the interfacial potential barrier by different mechanisms, such as thermionic emission, defect conduction, and quantum tunneling in the case of MS, MIS, and SIS moving structures. By tailoring the interface structure, it is possible to trigger electrical conduction resulting in optimized power output. We also show that the band bending in the surface-charged region of MoS2determines the direction of the dc power output. Our experimental results show that engineering the interface structure opens up new avenues for developing next-generation semiconductor-based mechanical energy conversion with high performance.