biocompatible, and biodegradable. However, inorganic piezoelectric materials are unsuitable for biological applications due to their inherent rigidity, fragility, and possible toxicity. Even those flexible piezoelectric organic polymers, for example, polyvinylidene difluoride (PVDF), are hard to meet many demands such as resorbability or degradability. [4] Piezoelectric biomaterials are promising alternatives since they naturally exhibit biocompatibility, reliability, and environmental sustainability. At present, the research on piezoelectric biomaterials is mainly focused on two types: piezoelectric biomolecules such as amino acids, peptides, virus, and cellulose, [5][6][7][8][9][10][11] and piezoelectric biological tissues like bone, wool, tendon, invertebrate exoskeletons, and epidermis. [12][13][14][15][16] However, due to the high cost and complexity of assembling and domain aligning the small biomolecules at a large scale, most of the research on their biological piezoelectricity is still at the theoretical level. [17] Additionally, because of the disorder of domains and the lack of ferroelectricity, biological tissues hardly exhibit piezoelectric properties at the macroscopic level, which limits the detection and application of their piezoelectricity. [18,19] Small intestinal submucosa (SIS) is the middle layer of small intestine, that supports the mucosa and joins it to the muscular layer. This material is one of the most extensively investigated scaffolds in both experimental and preclinical models for tissue repairing. SIS serves as a supporting scaffold to reconstruct various tissues such as tendon, arteriovenous tissues, and abdominal wall. [20,21] It has a great potential for versatile biomedical applications thanks to its biocompatibility and having no adverse response in cross-species transplantations. [22] In 1968, Fukada observed the direct piezoelectric effect in the intestines at the macroscale level. [23] However, the experimental quantitative determination of the intrinsic piezoelectric effect of SIS and the origin of its biological piezoelectricity have yet to be demonstrated due to its weak piezoelectricity at the macroscopic level and the limitation of measurement techniques. Although piezoresponse force microscopy (PFM) has been a powerful technique that allows quantitatively determining the piezoelectricity of biomaterials, [24,25] the thickness of the sample has a significant impact on the effective piezoresponses because the depth resolution of PFM is limited. [26,27] In addition, biological tissues hardly exhibit piezoelectricity at the thicker macroscopic level Piezoelectric biomaterials have attracted significant attention due to the potential effect of piezoelectricity on biological tissues and their versatile applications. However, the high cost and complexity of assembling and domain aligning biomolecules at a large scale, and the disordered arrangement of piezoelectric domains as well as the lack of ferroelectricity in natural biological tissues remain a roadblock toward practic...