Flexible, bio-compatible piezoelectric materials are of considerable research interest for a variety of applications, but many suffer from low response or high cost to manufacture. Herein, novel piezoelectric force and touch sensors based on self-assembled monolayers of oligopeptides are presented which produce large piezoelectric voltage response and are easily manufactured without the need for electrical poling. While the devices generate modest piezoelectric charge constants (d33) of up to 9.8 pC N −1 , they exhibit immense piezoelectric voltage constants (g33) up to 2 V m N −1. Furthermore, a flexible device prototype is demonstrated that produces open-circuit voltages of nearly 6 V under gentle bending motion. Improvements in peptide selection and device construction promise to further improve the already outstanding voltage response and open the door to numerous practical applications. Piezoelectric materials find use in a wide range of applications from touch and vibration sensors [1] to energy harvesters [2] to micromechanical actuators. [3] These devices rely on the piezoelectric effect to interconvert mechanical stress and electrical charge. In the direct piezoelectric effect, an applied force produces a resultant charge, whereas, in the converse effect, an applied voltage causes a mechanical deformation. Most existing piezoelectric materials are hard, brittle, leadcontaining ceramics such as lead zirconium titanate (PZT). [4] As such, these materials have limited ranges of motion, are liable to crack, and are not bio-compatible. While there is a large research focus on developing flexible, bio-compatible piezoelectric materials, [5] much of this work has involved placing traditional piezoelectrics on or into flexible substrates, often sacrificing electrical performance for added flexibility and ease of manufacturing (i.e., d-values <200 pC N −1 instead of 500 pC N −1-600 pC N −1 for PZT). [2,6,7] In addition to well known piezoelectric polymers such as semi-crystalline poly(vinylidene fluoride) (PVDF), researchers have begun to develop fundamentally new piezoelectric materials such as helicenes, amino acids, viruses, and peptides. [5,8-12]