LAUSR

Mesoporous single crystals combining the ordering of crystal lattice and the disordering of interconnected pores would create well‐defined structures confined at continuously twisted surfaces that are kinetically trapped. Here, mesoporous WN single crystal at 2 cm scale is grown to create and engineer the well‐defined surface structures. The unsaturated coordination structures including W–N1/2, W–N1/3, and W–N1/6 confined at twisted surfaces account for the chemisorption of H in acidic electrolyte and deliver a record high areal capacitance of ≈250 F cm−2 without degradation being observed even after 15 000 cycles. The engineering of well‐defined coordination structures at twisted surfaces would open an alternative to create active surfaces in the wealth of other single‐crystalline materials.