Energy barrier formed at a metal/semiconductor interface is a critical factor determining the performance of nanoelectronic devices. Although diverse methods for reducing the Schottky barrier height (SBH) via interface engineering have been developed, it is still difficult to achieve both an ultralow SBH and a low dependence on the contact metals. In this study, a novel structure, namely, a metal/transition-metal dichalcogenide (TMD) interlayer (IL)/dielectric IL/semiconductor (MTDS) structure, was developed to overcome these issues. Molybdenum disulfide (MoS2) is a promising TMD IL material owing to its interface characteristics, which yields a low SBH and reduces the reliance on contact metals. Moreover, an ultralow SBH is achieved via the insertion of an ultrathin ZnO layer between MoS2 and a semiconductor, thereby inducing an n-type doping effect on the MoS2 IL and forming an interface dipole in the favorable direction at the ZnO IL/semiconductor interfaces. Consequently, the lowest SBH (0.07 eV) and a remarkable improvement in the reverse current density (by a factor of approximately 5400) are achieved, with a wide room for contact-metal dependence. This study experimentally and theoretically validates the effect of the proposed MTDS structure, which can be a key technique for next-generation nanoelectronics.