Spider Webs‐Inspired Aluminum Coordination Hydrogel Piezoionic Sensors for Tactile Nerve Systems

Abstract Piezoionics, a new frontier that employs mobile ions as energy and charge carriers, plays an important role in new energy and intelligent electronics. However, a significant challenge consists in balancing the structural design of metal ions coordination hydrogel (HG‐MI) piezoionics for current conduction, voltage generation, and especially mechanical adaptability. Herein, inspired by the spider webs' unique structure, a strategy by realizing the full potential of metal‐ligand ions ([(OH)Cl 2 ] 3− ) to facilitate the keggin‐type structure AlOHAlOH generation together with activate functional carboxyls is introduced. Impressively, the whole property of the product HG‐Al PAC , especially the mechanical performance is improved. For example, the toughness of HG‐Al PAC is 2.75 MJ m −3 , more than twofold that of traditional HG‐Al AS/AC/AN samples. Due to the stable fixation of ─Al─OH─ thus promoting Cl − separation upon external force, HG‐Al PAC achieves a piezoionic coefficient of 0.89 mV KPa −1 and energy conversion efficiency of 1.29%, promising for mechanical‐electrical conversion and sensing. Combined with the good mechanical performance with the excellent piezoionic properties, underscores its potential as a tactile nerve system of analgesia patients to prevent them from being injured. This work intends to provide a stride toward mechanically robust self‐powered piezoionic sensors and offer insights into ionotropic materials for energy harvesting, human‐machine interaction, and biointerface.