Accurately calculated infrared spectra are essential for supporting experimental interpretation, yet full-space anharmonic vibrational structure calculations are only feasible for a limited number of degrees of freedom. Fortunately, characteristic spectroscopic signatures are often dominated by a few key vibrations. We propose a computational protocol specifically tailoring high dimensional anharmonic potential energy surfaces for the accurate and efficient calculation of such spectral signatures with vibrational coupled cluster response theory. Our protocol focuses on the selection of appropriate coordinates for the relevant degrees of freedom and the identification of specific mode-coupling terms for the potential energy surface that require more thorough treatment. This includes applying different levels of electronic structure theory and selecting a restricted set of higher mode-coupling terms (> mode pairs). We validate this protocol on two spectral regions: the fundamental CO stretching vibrations in uracil and the fundamental OH stretchings in catechol. Our findings indicate that the convergence behaviour towards harmonic frequencies in the so-called FALCON algorithm is an effective indicator for the locality character of the relevant degrees of freedom. We find that the CO stretchings in uracil are better described using normal coordinates, while the description with local FALCON coordinates of the OH-stretching vibrations in catechol showed superior performances in VCC spectra calculations. Overall, our protocol offers valuable guidelines for accurate and efficient anharmonic calculation of vibrational spectral signatures.