Interfacial design is one of the most promising ways in improving mechanical properties of nanocomposites.In this work,a multifunctional aerogel with excellent mechanical performances,sensing sensitivity,and fire retardancy is fabricated by taking advantage of metal coordination between biopolymer and Fe3+.Montmorillonite (MMT) nanosheets are added to induce a 'brick and mortar' structure.The coordination remarkably reduces structural defects,leading to well-formed lamellas that can effectively distribute stress under sever compression without plastic deformation.The structural merits impart the aerogel highly reversible compressibility even at 99 ％ strain and superior durability.Besides,it demonstrates high sensing performance in wearable health monitoring devices,and shows fire resistance property that can maintain elasticity in a flame.The work offers a facile and effective method to create multifunctional aerogels from various polymers.