Abstract Cyanides, ranging from three carbon atoms to polycyclic aromatic hydrocarbons, and alkenyl compounds are abundant in the interstellar medium. Aminoacrylonitrile (3-Amino-2-propenenitrile, H₂N–CH=CH–C≡N), an alkenyl cyanide, thus represents a promising candidate for new interstellar detection. A comprehensive spectroscopic laboratory investigation of aminoacrylonitrile in its rotational ground vibrational state has been herein performed. The measurements carried out up to the THz regime made it possible to generate a precise set of reliable rest frequencies for its search in space up to submillimeter wavelengths. The Z-aminoacrylonitrile (Z-apn) isomer spectrum has been recorded employing a source-modulated submillimeter spectrometer, from 80 GHz to 1 THz. A combination of Doppler and sub-Doppler measurement regimes allowed one to record 600 new lines. The collected data have enabled the characterization of a set of spectroscopic parameters up to decic centrifugal distortion constants. The catalog generated from the improved spectral data has been used for the search of Z-apn in the spectral survey of the G+0.693-0.027 molecular cloud located in the central molecular zone, in the proximity of the Galactic center.