Here, we report a novel class of electret-transducer materials developed by electrospinning copper indium disulfide (CuInS2) quantum dots (CIS-QDs), sulfonated cellulose nanocrystals (S–CNCs), and microbial polyhydroxybutyrate (PHB). The piezoelectret materials consist of CIS-QDs/S–CNCs/PHB-based highly-oriented electret fibers. The striking merits include large Stokes shifted red-luminescence, composting environment degradation, and dynamic self-polarization-enhanced piezoresponse. The first use of CuInS2-based QDs for doping in natural biopolymers suggests that the CIS-QDs allow for preferential orientation growth of piezoelectric phase PHB lamellae in bio-based electret fibers. The synergistic action of CIS-QDs-constrained, highly-oriented PHB micro-dipoles and dynamically-active S–CNCs macro-dipoles further enables a significantly enhanced piezoelectric response of the piezoelectrets. The piezoelectric output of red-emission CIS-QDs/S–CNCs/PHB-based nanogenerator is almost 2 and 5 times higher than that of S–CNCs/PHB-based and PHB-based devices, respectively. Moreover, the flexible self-powered device possesses the ability to collect and analyze athletic big data in intelligent sports. This class of versatile, ecologically decomposable piezoelectrets could be compelling building materials for applications in digital-twin- and metaverse-based ecosystems.