Good vibrations: Molecular vibrations with originally low or zero intensity in a vibrational circular dichroism (VCD) spectrum attain chirality in molecular crystals by coordinated motion of the atoms. Ab initio molecular dynamics simulations of anharmonic solid‐state VCD spectra of l‐alanine crystals reveal how coherent vibrational modes exploit the space group’s chirality, leading to non‐local, enhanced VCD features.