This thesis presents pioneering work in the relatively new field of focused ion beam (FIB) sculpting of single crystals to produce bespoke devices and enable the investigation of physics that cannot be studied in bulk samples. It begins with a comprehensive and didactic account of how to achieve this sculpting, revealing the ‘tricks of the trade’ of state-of-the-art FIB microstructuring. In subsequent chapters, the author presents ground-breaking results obtained from microstructures of the delafossite oxide metal PdCoO₂ and the heavy fermion superconductor...