Whereas mechanochemistry is rapidly advancing as a cleaner,faster and high yielding methodology for a vast range of chemical transformations,from organicsynthesis to making metal-organic frameworks,1 it also provides entirely new oportunities for the synthesis of materials or molecules.This presentation will outline some of our groups recent advances in the discovery of previously unknown chemical transformations for making active pharmaceutical ingredients and pharmaceutically attractive targets in general,2 as well as in the discovery of previously not known metal-organic frameworks.In particular,these synthetic advances are enabled solely through the application of mechanochemistry,and in some cases their development has been strongly aided through the application of recently introduced methodologies for real-time monitoring of mechanochemical milling reactions.3 The presented results will highlight the use of mechanochemistry and ball milling not only as a tool for greening chemical and materials synthesis,but as a self-standing tool for their development and discovery.