The correlation between the water and N-methylacetamide (NMA) intramolecular vibrational frequencies and the hydrogen-bond length in a variety of NMA-H₂O and NMA-D₂O complexes was investigated by carrying out ab initio calculations. As the hydrogen-bond length decreases, the frequencies of bending and stretching modes of the hydrogen-bonding water increases and decreases, respectively, and the amide I and II (III) mode frequencies of the NMA decreases and increases, respectively. In this paper, correlation maps among the amide (I, II, and III) modes of NMA and three intramolecular water modes are thus established, which in turn can be used as guidelines for interpreting two-dimensional vibrational spectra of aqueous NMA solutions.