Summary Low thermal conductivity of metal-organic frameworks (MOFs) restricts their kinetic performance when used in thermal-relevant fields. A facile and straightforward manufacturing method, laser shock-induced evaporation, is devised here to deposit uniform liquid metal nanoparticle (LMNP) thin layers on the surface of MOF crystals, resulting in MOF@LMNP nanocomposites. Localized evaporation induced by selective laser absorption in liquid metal fragments the liquid metal particles and deposits them as thin layer on MOF surfaces. The LMNP layer acts as a 3D heat-conductive highway that boosts the thermal conductivity of MOF@LMNP up to five times compared with pristine MOFs. After the measurement of the atmospheric water harvest capability, the composite could rapidly release the absorbed water and doubles the water productivity in 3 min by enhancing the heat transfer and accelerating the kinetics for water release.