Nitriles constitute almost 20% of the molecules observed in the interstellar medium, whereas only one dinitrile and one isocyanonitrile compound have been detected up to now. The lack of detections of such compounds may be partially explained by the lack of accurate spectroscopic data on their rotational spectra. Two small seven-atom dinitriles, malononitrile NCCH_2_CN and isocyanoacetonitrile NCCH_2_NC, were chosen as target species for this study. For malononitrile the goal of the study is to systematize all the previous measurements, and to extend the measurements to the sub-millimeter wavelength range. The spectrum of isocyanoacetonitrile has not been studied before. The rotational spectra of the two molecules was measured in the frequency range 150-660GHz using the Lille fast-scan spectrometer. The spectroscopic study was supported by high-level theoretical calculations on the structure of these molecules and their harmonic force field. Accurate frequency predictions for malononitrile and isocyanoacetonitrile were calculated on the basis of the analysis of their rotational spectra. The influence of the spin statistics on the intensities of the lines of malononitrile was taken into account. The provided line lists and sets of molecular parameters meet the needs of astrophysical searches for the two molecules.