Achieving the Upper Bound of Piezoelectric Response in Tunable,Wearable 3D Printed Nanocomposites

The trade‐off between processability and functional responses presents significant challenges for incorporating piezoelectric materials as potential 3D printable feedstock. Structural compliance and electromechanical coupling sensitivity have been tightly coupled: high piezoelectric responsiveness comes at the cost of low compliance. Here, the formulation and design strategy are presented for a class of a 3D printable, wearable piezoelectric nanocomposite that approaches the upper bound of piezoelectric charge constants while maintaining high compliance. An effective electromechanical interphase model is introduced to elucidate the effects of interfacial functionalization between the highly concentrated perovskite nanoparticulate inclusions (exceeding 74 wt%) and light‐sensitive monomer matrix, shedding light on the significant enhancement of piezoelectric coefficients. It is shown that, through theoretical calculation and experimental validations, maximizing the functionalization level approaches the theoretical upper bound of the piezoelectric constant d₃₃ at any given loading concentration. Based on these findings, their applicability is demonstrated by designing and 3D printing piezoelectric materials that simultaneously achieve high electromechanical sensitivity and structural functionality, as highly sensitive wearables that detect low pressure air (<50 Pa) coming from different directions, as well as wireless, self‐sensing sporting gloves for simultaneous impact absorption and punching force mapping.