The α-aminonitrile, 2-morpholino-2-(3,4,5-trimethoxyphenyl)acetonitrile (C15H20N2O4), was prepared through a silica sulfuric acid-catalyzed Strecker reaction between 3,4,5-trimethoxybenzaldehyde, morpholine, and two different cyanide sources. Molecular characterization was performed by Fourier transform infrared spectroscopy, gas chromatography–mass spectrometry, (1H, 13C – mono and bidimensional) nuclear magnetic resonance; crystallographic characterization was completed by X-ray powder diffraction of polycrystalline samples. The title compounds crystallized in a monoclinic system and unit-cell parameters are reported [a = 13.904(2), b = 5.1696(6), c = 21.628(3) Å, β = 104.31(1)°, unit-cell volume V = 1506.3(3) Å3, Z = 4]. All measured lines were indexed with the P21/a (No. 14) space group.