Doping-induced local symmetry breaking of centrosymmetric molecular crystals endows them with piezoelectric and pyroelectric properties. In this work, we measured temperature dependences of pyroelectric and piezoelectric coefficients in α-glycine crystals single-doped by threonine and double-doped by threonine and alanine. We analyzed primary and secondary pyroelectric effects in these crystals and suggested a model of the dopant complexes related to the observed effects. © Pleiades Publishing, Ltd. 2023.