Understanding segregation to grain boundaries and their effects on GB cohesion is critical to enabling rational grain boundary engineering for alloys design. Here, we discuss the progress and challenges one may face when generating such a database of defect-solute interactions, in the context of studying of grain boundary segregation of solutes and impurities in Ni GBs. To compute the large number of relevant defect-solute interactions we have performed high-throughput ab initio calculations using efficient and highly automated workflows using pyiron, an open-source toolkit for materials science. The study has been performed across a representative set of coincident-site-lattice (CSL) type tilt GBs. Based on the large ab-initio datasets, we extract and analyse the chemical and structural trends observed in the solute segregation behaviour across the periodic table. The features which are most important in evaluating site segregation are presented and discussed.