An　efficient　technique　using　citric　acid　and　glucose　based　natural　deep　eutectic　solvent　(G-C-NADES)　was　developed　to　obtain　ultrahigh　deamidated　wheat　gluten　(UDWG)　(deamidation　degree　(DD)　＞　90%).　FTIR　and　1H　NMR　indicated　intensive　hydrogen　bonds　(HBs)　in　G-C-NADES　supermolecules.　Quantum　chemical　calculations　and　molecular　dynamic　simulations　demonstrated　that　10　wt　%　diluted　G-C-NADES　still　had　a　myriad　of　HBs.　Physicochemical　results　showed　UDWG　had　DD　up　to　92.45%　after　G-C-NADES　deamidation,　that　is,　22%　higher　than　citric-acid-DWG　with　a　weak　degree　of　hydrolysis　(1.75%).　Conformational　characterization　demonstrated　the　obvious　conversion　from　α-helix　to　β-sheet　via　FTIR,　the　least　amount　of　disulfide　bonds　by　Raman　spectra,　and　more　exposure　of　tryptophan　residues　by　fluorescence　measurement　for　UDWG.　It　is　proven　that　enhanced　accessible　conformation　of　WG　reached　with　HBs　of　G-C-NADESs　could　contribute　to　the　improvement　on　nucleophilic　attack　of　deamidation,　declaring　that　G-C-NADES　might　be　a　potential　solvent　for　obtaining　an　ultrahigh　deamidation　for　WG　to　successfully　guarantee　the　safety　of　wheat　gluten　based　cereal　food　regarding　to　lowering　its　allergy.　©　2021　American　Chemical　Society.