Cocrystallization
of two or more molecular compounds can dramatically
change the physicochemical properties of a functional molecule without
the need for chemical modification. For example, coformers can enhance
the mechanical stability, processability, and solubility of pharmaceutical
compounds to enable better medicines. Here, we demonstrate that amino
acid cocrystals can enhance functional electromechanical properties
in simple, sustainable materials as exemplified by glycine and sulfamic
acid. These coformers crystallize independently in centrosymmetric
space groups when they are grown as single-component crystals but
form a noncentrosymmetric, electromechanically active ionic cocrystal
when they are crystallized together. The piezoelectricity of the cocrystal
is characterized using techniques tailored to overcome the challenges
associated with measuring the electromechanical properties of soft
(organic) crystals. The piezoelectric tensor of the cocrystal is mapped
using density functional theory (DFT) computer models, and the predicted
single-crystal longitudinal response of 2 pC/N is verified using second-harmonic
generation (SHG) and piezoresponse force microscopy (PFM). The experimental
measurements are facilitated by polycrystalline film growth that allows
for macroscopic and nanoscale quantification of the longitudinal out-of-plane
response, which is in the range exploited in piezoelectric technologies
made from quartz, aluminum nitride, and zinc oxide. The large-area
polycrystalline film retains a damped response of ≥0.2 pC/N,
indicating the potential for application of such inexpensive and eco-friendly
amino acid–based cocrystal coatings in, for example, autonomous
ambient-powered devices in edge computing.