Ni-based superalloys have excellent high-temperature properties including strength, making them key alloys for high-temperature turbine blades in modern aircraft. Modern Ni-based superalloys are directionally cast as single crystals. During solidification, dendrites form due to thermodynamic preferences of alloying elements to partition into different phases. The extent of the partitioning of elements into different phases can affect mechanical properties and subsequently affect alloy performance and engine lifetime. The demanding conditions these alloys are exposed to can affect element behaviour and partitioning. Continued development of these alloys requires an atomic-level understanding of the origins and evolution of the microstructure that is sustained during initial processing and subsequent exposure to harsh environments. My PhD looks at mapping these origins and evolutions in a series of alloys from different conditions using atom probe tomography and other complementary techniques.