In this work, we assess the AIMD-based approach for ac-curately predicting IR and Raman spectra of layered 2D materials. Our goal is to develop a computational tool to support the interpretation of in situ vibrational spectroscopy during wet-chemical synthesis of layered COFs and similar porous materials. We focus thus on host-guest interactions between the framework material and solvent molecules and strategies for analyzing the AIMD-based spectra. We demonstrate how to dissect the AIMD-based spectra into individual contributions from the solvent, the molecular units of the framework material, and the covalent bonds connecting these molecular units. Identifying and monitoring the vibrational bands related to these connecting bonds is crucial for verifying the successful synthesis of the framework material. Specifically, we investigate the COF-1 system with and without 1,4dioxane solvent molecules in the pores. We propose computationally robust settings to obtain AIMD-based IR and Raman spectra for COF-1 and demonstrate how to dissect the spectra by adapting established strategies. We expect that the majority of our findings are transferable to other framework materials.