Sophisticated microelectromechanical systems for device and sensor applications have flourished in the past decade. These devices exploit piezoelectric, capacitive, and piezoresistive effects, and coupling between them. However, high-performance piezoresistivity (as defined by on/off ratio) has primarily been observed in macroscopic single crystals.1 In this Letter, we show for the first time that rare-earth monochalcogenides in thin film form can modulate a current by more than 1000 times due to a pressure-induced insulator to metal transition. Furthermore, films as thin as 8 nm show a piezoresistive response. The combination of high performance and scalability make these promising candidates for nanoscale applications, such as the recently proposed piezoelectronic transistor (PET).2,3 The PET would mechanically couple a piezoelectric thin film with a piezoresistive switching layer, potentially scaling to higher speeds and lower powers than today's complementary metal-oxide-semiconductor technology. © 2013 American Chemical Society.