FT-IR spectra were recorded on a Bruker Vertex 70 FT-IR instrument in the range from 400 cm -1 to 4000 cm -1 in attenuated total reflectance (ATR) mode. For the measurements, the ATR diamond of the spectrometer was covered with the sample, using approximately 1-2 mg of sample. All measurements were background corrected. Raman measurements were performed on a Bruker RFS 100 FT-Raman spectrometer with a 1064 nm laser and a liquid N 2 -cooled Ge-detector. The spectra were background corrected and performed at λ=1064 nm with a resolution of 4 cm -1 and 800-1000 mW power (100 scans). For measurement, the sample was packed in a soda lime glass capillary (1.50 mm outer diameter, 1.20 mm inner diameter) inside an Ar-filled glovebox. Details on the PXRD and physisorption measurements are given in Section S3 in the SI, together with the obtained PXRD spectra (Figure ) and N 2 adsorptiondesorption isotherms (Figure ) for COF-1.