Fluoropolymers, including polytetrafluoroethylene (PTFE, Teflon), polyvinylidene difluoride (PVDF), and fluorine kautschuk materials (FKMs, Viton) are critical polymers for applications ranging from non‐stick coatings, corrosion resistant seals, semiconductor manufacturing, membranes, and energy harvesting technologies. However, the synthesis of these fluoropolymers requires the use of per‐ and polyfluorinated alkyl substances (PFAS) known colloquially as “forever chemicals,” and as such there is a pressing need to develop alternative technologies that can serve the end‐use of fluoropolymers without the environmental cost of using PFAS. Further, fluoropolymers themselves fall under the PFAS umbrella. Here, alternative mechanical‐to‐electrical energy harvesting polymers are reviewed and benchmarked against the leading fluoropolymer energy harvesters. These alternative technologies include nonfluoropolymer piezoelectric polymers, triboelectric nanogenerators (TENGs), ferroelectric elastomers, and flexoelectric polymers. A vision towards sustainable, non‐fluoropolymer‐based energy harvesting is provided.