Further support for our HB geometry-based ∆𝜈̅ 𝐻𝐵, (𝑑, 𝜃) model and the observation of large values for head-on and/or short HBs is provided by a new publication where a nitrile probe was incorporated into different metal organic frameworks (MOFs). The rigid MOF structure enabled the introduction of H-bonding moieties (allylic and aromatic carboxylic acids) near the nitrile. According to DFT, these C≡N---HO interactions occur at average HB and, respectively. The bottom row shows corresponding MD-based simulated IR spectra using eq. 2 (with eqs. 1a and 7) and parameters in Table (and Table ) as a vibrational spectroscopic map (vsm) obtained using the fluctuating frequency approximation (see Methods Section). The solid red vertical lines are predicted peak positions due to the VSE only (using eq. 1b and parameters from ref. ) in Fig. and, and the blueshifts derived from the vsm (∆𝜈̅ 𝐻𝐵,𝑣𝑠𝑚 ) are the difference between the simulated peak position and the frequency of the red line. Data in A is reproduced from ref. . Copyright 2022 American Chemical Society. distances/angles of 2.85 Å/168° (allylic acid; "AA"), 2.80 Å/148° (benzoic acid; "CPh"), and 2.79 Å/150° (isophthalic acid; "DCPh"). As in the case of F92oCNF, ∆𝜈̅ 𝐻𝐵,𝑜𝑏𝑠 and 〈∆𝜈̅ 𝐻𝐵, (𝑑, 𝜃)〉 are in excellent agreement: the experimental/predicted values (in cm -1 ) for AA are 36/31.8, for CPh are 29/28.2, and for DCPh are 33/32.2. It is interesting to note that the nitrile in the MOFs is an aliphatic C≡N, not an oTN derivative, and that the nitrile HB partners are carboxylic acids, not water or alcohols. These differences make the similarity between the experimental and our predicted HB shifts all the more impressive; this comparison suggests that our model can work generally for H-bonded nitriles with different types of HB donors.