An interaction between methyl torsion and the low-lying out-of-plane methyl wag vibration has been observed in toluene, p-fluorotoluene, and m-fluorotoluene, contravening the traditional assumption used when analyzing spectra that methyl torsion can be treated independently of the small-amplitude vibrations. When a methyl group is attached to a planar frame, out-of-plane methyl wag vibrations always occur, and hence this type of interaction between methyl torsion and vibration is potentially extensive. To probe whether this coupling occurs beyond toluene and its derivatives, we have studied the far-infrared absorption band for the out-of-plane methyl wagging mode in N-methylpyrrole. The torsional sequence structure reveals a particularly strong torsion-vibration interaction. Spectral simulations yield a torsion-vibration coupling matrix element of 34.0 cm-1, over twice the value for toluene. The large torsion-vibration coupling constant implies that there is a significant tilting of the methyl group out of plane. Quantum chemistry calculations reveal a much larger out-of-plane methyl tilt angle in N-methylpyrrole compared to toluene, qualitatively consistent with this expectation. This is the first nontoluene derivative for which this type of torsion-vibration interaction has been reported and shows that the effect extends beyond toluenes. When present, this interaction links small-amplitude vibrations to the methyl torsion, providing a mechanism to bring the increased density of states into play and accelerate the rate of intramolecular vibrational energy redistribution.