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Modified organic silica sol coating was prepared on the surface of zirconium hydride (ZrH1.8) by sol-gel technology using ethyl silicate (TEOS), isopropyl alcohol (IPA) and H2O as raw materials, coupling agent 3-methacryloxypropyltrimethoxysilane (KH570) and vinyl trimethoxy silane (A171) and H3PO4 as modifier agent.FTIR analysis showed that modifier agent could participate in copolymerization reaction of the sol effectively.TEM analysis showed that its advantageous to refine colloidal particle size as KH570 and A171 were added.Space network structure sol was formed as H3PO4 added for its improved the affinity between colloidal particles.SEM analysis showed that dried coating on ZrH1.8 substrate prepared by sol-gel dip-coating method was crack-free.After sintered in CO2 atmosphere under intermediate sintering temperature, the coating appeared micro-cracks, however, without severe fragmentation.Uniform and crack-free in situ oxidation layer was prepared on the surface of ZrH1.8 substrate as the sol coating played a buffer role for the oxygen diffusion in sintering process.Thermal hydrogen release experiment in vacuum demonstrated that sintered sol coating cooperate with in situ oxidation layer on ZrH1.8 could resistant hydrogen permeation.