This dataset contains biolayer interferrometry raw data as a Supplement to the manuscript (Nature Chemistry manuscript NCHEM-25113756A) "An artificial protein-foldamer supramolecular synthon for self-assembled hybrid architectures" in form of their respective experiment folders of the Octet system for easy access in Octet Analysis Studio directly. The folders also contain the respective result files in .csv format. In addition the folder contains the source mass spectrometric, size exclusion chromatography and circular dichroism data that served to make the graphs in Figures 1, 2 and 3 of the manuscript. These are provided in .csv format.eng