Graphite carbons have been widely used as catalyst support due to their low‐cost, tunable porous structure, high electrical conductivity, and good resistance to harsh conditions. To date, various defect engineerings have been adopted to enhance the cohesion between graphite carbons and metallic nanocatalysts. Nevertheless, the modification of carbon basal plane has been less explored. In this work, a dual modification strategy is developed to achieve novel carbon support (denoted as NCf) incorporating both C60 units and trace N‐defects. Benefiting from the dual anchoring modes (Ru–C and Ru–N–C), ultrafine ruthenium (Ru) nanoclusters (average size: 2.26 ± 0.38 nm) can be well‐dispersed and robustly anchored on the NCf support. The optimal Ru0.013@NCf catalyst exhibits decent catalytic activities and long‐term stabilities toward both alkaline hydrogen evolution reaction (HER) and aromatic nitroreduction (ANR), outperforming the individually modified counterparts. Computational studies suggest that introducing both C60 and N‐defects into carbon support leads to electron‐deficient Ru nanocluster, which is critical for not only HER but also ANR. This work thus provides a new guideline for rational design of advanced carbon supported nanocatalysts for multipurpose applications.