Modulating the orientation of piezoelectric crystals in biomolecules to match the varying mechanical environments in the body and achieve optimal efficiency remains a key challenge for their biomedical applications. Here, we successfully developed a molecular self-assembly approach to fabricate flexible piezoelectric Glycine-Nb2CTx (Gly-Nb2C) films with crystal orientations ranging from 6 degrees to 82 degrees, modulated by Nb2CTx nanosheets. The GlyNb2C films exhibited crystal orientation-dependent macroscopic longitudinal and transverse piezoelectric properties, as well as rapid NIR photothermal conversion, increasing from 28 degrees C to 43 degrees C within 3 min. These properties facilitate efficient electromechanical sensing capabilities, enabling targeted applications in distinct mechanical environments in vivo, such as the longitudinal forces in the pectoral muscle and the transverse forces in the quadriceps femoris. Ultimately, the Gly-Nb2C film was employed as an electronic patch to effectively promote skin wound regeneration. The synergistic effect of transverse electric stimulation and appropriate heat significantly reduced inflammation and promoted skin cell growth, thereby enhancing both re-epithelialization and vascularization. The unique multifunctional properties of multi-directional piezoelectricity, rapid photo-thermal response, and biodegradability, combined with the simplicity and versatility of its manufacturing process, make this film highly promising for biomedical applications.