Aqueous　zinc-ion　batteries　(AZIBs)　are　promising　large-scale　energy　storage　devices　due　to　their　costeffectiveness　and　high　safety.　However,　the　rampant　dendrite　growth　and　notorious　side　reactions　resulting　from　the　decomposition　of　active　water　molecules　hinder　its　practical　application.　Herein,　the　zincophilic　polyoltype　surfactant　of　alkyl　polyglycoside　(APG)　is　introduced　to　induce　the　rearrangement　of　the　H-bonds　network　to　diminish　the　free　water　activity,　facilitating　the　zinc-ion　solvation　structure　transition　from　[Zn2+(H2O)6　&　sdot;SO42-]　(solvent　separated　ion　pair,　SSIP)　to　[Zn2+(H2O)5　&　sdot;OSO32-]　(contact　ion　pair,　CIP)　with　less　Zn2+-solvated　H2O.　Meanwhile,　the　APG　molecular　preferentially　adsorb　on　the　Zn　surface　to　form　a　dehydrated　layer,　which　can　suppress　the　hydrogen　evolution　reaction　(HER)　and　hinder　the　two-dimensional　(2D)　diffusion　of　Zn2+　ions.　Consequently,　the　Zn//Zn　symmetric　cell　using　our　designed　electrolyte　demonstrates　an　ultralong　cycle　life　of　5250　h　at　1.0　mA　cm-2/1.0　mAh　cm-2.　Furthermore,　the　as-prepared　Zn//Na2V6O16　&　sdot;3H2O　full　cell　also　delivers　a　high-capacity　retention　rate　of　80.8%　even　after　1000　cycles　at　2.0　A　g-1,　superior　to　that　of　the　full　cell　using　pure　ZnSO4　electrolyte.　This　study　offers　an　effective　strategy　to　modulate　the　cation　solvation　structure　by　rearranging　the　H-bonds　network　for　a　highly　reversible　Zn　anode.