Ionogels　have　garnered　significant　interest　due　to　their　great　potential　in　flexible　iontronic　devices.　However,　their　limited　mechanical　tunability　and　environmental　intolerance　have　posed　significant　challenges　for　their　integration　into　next-generation　flexible　electronics　in　different　scenarios.　Herein,　the　synergistic　effect　of　cation-oxygen　coordination　interaction　and　hydrogen　bonding　is　leveraged　to　construct　a　3D　supramolecular　network,　resulting　in　ionogels　with　tunable　modulus,　stretchability,　and　strength,　achieving　an　unprecedented　elongation　at　break　of　10 800%.　Moreover,　the　supramolecular　network　endows　the　ionogels　with　extremely　high　fracture　energy,　crack　insensitivity,　and　high　elasticity.　Meanwhile,　the　high　environmental　stability　and　hydrophobic　network　of　the　ionogels　further　shield　them　from　the　unfavorable　effects　of　temperature　variations　and　water　molecules,　enabling　them　to　operate　within　a　broad　temperature　range　and　exhibit　robust　underwater　adhesion.　Then,　the　ionogel　is　assembled　into　a　wearable　sensor,　demonstrating　its　great　potential　in　flexible　sensing　(temperature,　pressure,　and　strain)　and　underwater　signal　transmission.　This　work　can　inspire　the　applications　of　ionogels　in　multifunctional　sensing　and　wearable　fields.　©　2024　Wiley-VCH　GmbH.