Covalently Aligned Molybdenum Disulfide–Carbon Nanotubes Heteroarchitecture for High‐Performance Electrochemical Capacitors

Abstract Advanced two‐dimensional nanosheets that promote the dynamic transportation and storage capacity of ions are significant for high‐performance electrochemical capacitors (ECs). However, such materials often possess a low energy density. We have developed an ordered heteroarchitecture of molybdenum disulfide‐carbon nanotubes (MoS 2 ‐CNTs) in which CNTs are vertically grafted within a MoS 2 framework by C−Mo covalent bonds. Benefiting from this in situ vertical bridge, high‐speed interlaminar conductivity, unimpeded ion‐diffusion channels and sufficient pseudocapacitive reactivity, the MoS 2 ‐CNTs presents ultralarge capacitance (5485 F g −1 ) and good structural stability in potassium hydroxide electrolyte. Moreover, the all‐unified solid‐state flexible ECs obtained through direct‐write printing construction deliver high energy density (226 mWh g −1 ), good capacitance (723 F g −1 ) and stable high/low‐temperature operating ability, which can power a wearable health‐monitoring device.