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 [email protected] 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 [email protected] 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.