Binders　play　an　important　role　in　preserving　the　mechanical　stability　of　electrodes.　Nevertheless,　the　typical　binders　normally　are　not　stretchable　to　withstand　a　repeated　large　volume　change,　which　are　not　suitable　for　high-loading　silicon　anodes.　Herein,　inspired　by　the　natural　parthenocissus,　an　elastic　self-healing　CA-PAA　binder　is　designed　for　silicon　anode　to　implement　long-terms　stable　cycling.　The　multiple　hydrogen　bonds　formed　by　in-situ　cross-linking　of　water　soluble　citric　acid　(CA)　and　poly　(acrylic　acid)　(PAA)　can　establish　a　reversible　network　for　silicon　particles.　The　CA　molecule　not　only　serves　as　the　protecting　buffer　layer　to　release　the　inner　stress　and　stabilize　the　solid　electrolyte　interface　(SEI),　but　it　can　also　connect　with　PAA　to　form　a　＇inner　flexibility　and　outer　rigidity＇　spatial　topology.　Consequently,　this　self-healing　binder　enhanced　silicon　anode　exhibits　an　excellent　performance　on　accommodating　the　large　volume　change　during　cycling　process.　As　expected,　the　silicon　anode　shows　an　impressive　initial　areal　capacity　of　6.5　mAh　cm−2,　78%　capacity　retention　after　50　cycles　with　a　high　mass　loading　of　1.8　mg　cm−2,　and　an　initial　Coulombic　efficiency　of　89.5%.　Meanwhile,　the　Si||NCM811　full　cell　shows　74%　capacity　retention　after　100　cycles　with　a　reversible　capacity　of　1.7　mAh　cm−2.　©　2021