Advanced two-dimensional nanosheets that promote the dynamic transportation and storage capacity of ions are significant for high-performance electrochemical capacitors (ECs). However,s uch materials often possess al ow energy density.W eh ave developed an ordered heteroarchitecture of molybdenum disulfide-carbon nanotubes (MoS 2 -CNTs) in which CNTs are vertically grafted within aM oS 2 framework by CÀMo covalent bonds.B enefiting from this in situ vertical bridge,h igh-speed interlaminar conductivity,u nimpeded iondiffusion channels and sufficient pseudocapacitive reactivity, the MoS 2 -CNTs presents ultralarge capacitance (5485 Fg À1 ) and good structural stability in potassium hydroxidee lectrolyte.Moreover,the all-unified solid-state flexible ECs obtained through direct-write printing construction deliver high energy density (226 mWh g À1 ), good capacitance (723 Fg À1 )and stable high/low-temperature operating ability,w hich can power aw earable health-monitoring device.