This dataset contains the raw and processed experimental data supporting the results presented in the thesis titled "Non-Covalent Surface Modification of Proteins Using Guanidinium-Based Molecular Glues". It includes data from a range of experimental techniques, such as UV–Vis spectroscopy, enzyme kinetic assays, fluorescence experiments, ESI-MS, NMR, TEM imaging, cell viability assays, as well as other supporting experiments. The study establishes molecular design frameworks for guanidinium-based noncovalent protein surface modification, with applications in intracellular protein delivery, therapeutic modulation, and real-time visualization.