Large Enhancement on Performance of Flexible Cellulose‐Based Piezoelectric Composite Film by Welding CNF and MXene via Growing ZnO to Construct a “Brick‐Rebar‐Mortar” Structure

Abstract Cellulose‐based piezoelectric composites have attracted extensive attention in recent years due to their low cost, easy molding, high flexibility, and biocompatibility in the manufacture of piezoelectric nanogenerators (PENG) and sensors. In this work, cellulose nanofibril (CNF)/MXene@ZnO (CM@ZnO) piezoelectric composite films with “brick‐rebar‐mortar” structure are prepared by growing ZnO on the mixed substrate via a high‐efficiency two‐step hydrothermal method. As a hard bridge, ZnO welds CNF and MXene together to construct the “brick‐rebar‐mortar” structure, which greatly improves the piezoelectric performance. Its tensile strength reaches 65.13 ± 3.61 MPa, as well as that the longitudinal piezoelectric constant (d₃₃) attains 14.3 ± 1.3 pC N⁻¹. Under the force of 300 KPa, the open‐circuit voltage (V_OC) and short‐circuit current (I_SC) of CM@ZnO PENG are as high as 17.15 V and 997 nA, respectively. Under the force of 100 KPa, it can charge a 1.0 µF commercial capacitor to 6.07 V in 400 s. The assembled flexible piezoelectric sensor can accurately collect the pressure or vibration signal caused by bending the wrist (0.59 V) with excellent sensitivity. The performance demonstrates the feasibility of its application in wearable smart devices and provides a reference for new cellulose‐based PENGs.