The　poor　cycling　stability　of　aqueous　zinc-ion　batteries　(AZIBs),　caused　by　zinc　dendrite　growth　and　surface　corrosion-induced　passivation　at　the　zinc　anode,　significantly　hinders　their　practical　development.　In　this　work,　7-(2,3-dihydroxypropyl)theophylline　(DHTP)　is　introduced　as　a　functional　additive　into　Zn(CF3SO3)2　(ZOT)　electrolyte　to　regulate　the　anode-electrolyte　interface　and　mitigate　side　reactions.　Theoretical　calculations　and　experimental　characterizations　reveal　that　DHTP　preferentially　adsorbs　on　the　zinc　anode,　reducing　direct　water　contact　and　thereby　suppressing　hydrogen　evolution　and　corrosion　reactions.　Notably,　DHTP　exhibits　the　lowest　adsorption　energy　on　the　Zn(002)　crystal　plane,　which　optimizes　Zn2+　diffusion　and　deposition　behavior,　guiding　the　preferential　growth　of　the　Zn(002)　plane.　Benefiting　from　this,　the　Zn||Zn　symmetric　cell　with　DHTP　achieves　stable　cycling　for　over　800　h　at　1　mA　cm−2　and　1　mAh　cm−2,　outperforming　the　bare　electrolyte.　Furthermore,　the　Zn||NaV3O8·1.5H2O　full　cell　demonstrates　exceptional　durability　of　9,000　cycles　with　a　remarkable　capacity　retention　of　89　%　under　a　high　current　density　of　10　A　g−1.　This　molecular　adsorption　strategy　based　on　DHTP　provides　a　novel　approach　to　constructing　highly　reversible　zinc　anodes　for　advanced　AZIBs.　©　2025