The microwave spectra of the two isotopes ('3CH3'2C15N and 13CH313C1SN) of the methyl cyanide molecule in the 3 u s , U, and v4 vibrational energy levels for the rotational components 1 s J s 5 (for a range of frequencies 17-95 GHz) were experimentally and theoretically examined. Rotational components in each vibration were measured to determine the mutual interactions in each vibration investigated.The method of isotopic substitution was employed for internal tuning of each vibrational level by single and double substitution of 13C in the two sites of the molecule. It was found that relative frequencies within each vibration with respect to another vibration were shifted in a systematic way. The results given in this work were interpreted on the basis of these energy shifts. Large departures between experimentally measured and theoretically predicted frequencies for the quantum sets ( J , K = *l, I = i l ) , KI = 1 in the 3us and U, vibrational states in 13CH3'2C'SN and 13CH3'3C'SN showed anomalous behaviour which was explained as being due to a Fermi resonance between these vibrational modes.