 Piezoelectric biomaterials are gaining popularity due to their potential applications in implantable sensors, actuators, and energy harvesters. However, their practical use has been limited by the weak piezoelectric effect, caused by the random polarization of biomaterials and the difficulty of achieving large-scale domain alignment. To overcome these limitations, researchers developed an active self-assembly strategy to tailor piezoelectric biomaterial films. By confining the material within nanoscale pores, they were able to achieve homogeneous nucleation of crystals across the entire film, resulting in an enhanced piezoelectric strain coefficient of 11.2 pm of E1 and an exceptionally high piezoelectric voltage coefficient of 252x10 to 3 vmn1. Furthermore, this technique also improved the thermo-stability of the material, making it suitable for biomedical devices. This article was authored by Zhueming Zhong, Xuemu Li, Zhou Wapeng, and others.