Unlocking the Ultrahigh‐Current‐Density Hydrogen Evolution on 2H‐MoS₂ via Simultaneous Structural Control across Seven Orders of Magnitude

Abstract Members of transition metal dichalcogenides, particularly molybdenum disulfide, have been recognized as promising efficient and durable earth‐abundant catalysts for the hydrogen evolution reaction (HER). Despite the recent significant progress, the HER performance of MoS₂ is still far from satisfactory, especially at high current densities. Here, a simultaneous multilevel structural control strategy is reported to cooperatively boost hydrogen evolution on 2H‐MoS₂, unlocking its potential for practical hydrogen evolution at ampere‐level current densities. By confining the epitaxial growth of few‐layered, curved MoS₂ nanosheets within a tubular mesoporous graphitic framework, one can achieve deliberate structural control of MoS₂ across seven orders of magnitude on the length scale. The resulting MoS₂@C supertubes, benefiting from their unique structural features across atomic‐to‐microscopic scales, are characterized by abundant edge sites and sulfur vacancies, facilitated charge and mass transport, and rapid gas bubble removal. As a consequence, such MoS₂@C supertubes exhibit exceptional high‐current‐density HER activity surpassing previously reported 2H‐MoS₂ catalysts and even commercial Pt/C catalysts. This work demonstrates the validity of multilevel structural engineering of 2H‐MoS₂ by confinement growth, opening a viable route of developing low‐cost catalysts toward practical hydrogen evolution.