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Organic-inorganic material hybridization at the solid-state level is indispensable for the integration of IoT applications, but still remains a challenging issue. Existing bonding strategies in the field of electronic packaging tend to employ vacuum or ultrahigh temperature; however, these can cause process complications and material deterioration. Here we report an easy-to-tune method to achieve hybrid bonding at the solid-state level and under the ambient atmosphere. Vacuum-ultraviolet (VUV)-induced reorganization with ethanol was used to develop hydroxyl-carrying alkyl chains through coordinatively-bonded carboxylate onto aluminum, whereas numerous hydroxyl-carrying alkyls were created on polyimide. The triggering of dehydration through these hydroxyls by merely heating at 150 °C for a few minutes produced robust organic-inorganic reticulated complexes within the aluminum/polyimide interface. The as-bonded aluminum/polyimide interface possessed an superior fracture energy of (2.40 ± 0.36) × 10 3  (J/m 2 ) compared with aluminum and polyimide matrices themselves, which was mainly attributed to crack deflection due to the nano-grains of inorganic-organic reticulated complexes. The interfacial adhesion was successfully kept after humidity test, which was contributed by those anti-hydrolytic carboxylates. To the best of our knowledge, for the first time organic-inorganic bonding at the solid-state level was achieved using the ethanol-assisted VUV (E-VUV) process, a strategy which should be applicable to a diversity of plastics and metals with native oxides.

Organic-Inorganic Solid-State Hybridization with High-Strength and Anti-Hydrolysis Interface