A dual-layered shells/core microcrystal (graphene-oxide (GO)-titanium-dioxide (TiO2)/sodium-chloride (NaCl), GTNC) is synthesized by evaporation crystallization. After thermal reduction, an alternating hydrophilic (TiO2 nanoparticles)/hydrophobic (rGO plates) nanostructure is formed, sharing similarities to the water-vapor-harvesting system of desert beetles. rGTNC microcrystals could deliquesce at lower relative humidity (59 +/- 3%, RH) than that of NaCl (similar to 75% RH), and form larger water droplets similar to 4-8 times its original areal size. The enhanced performance is attributed to surface energy gradients and water adsorbing capability. The results confirm that rGTNC microcrystals can be used as efficient cloud seeding materials.