This research investigates innovative compositional applications of microtonal musical techniques to locate new expressive dimensions in music. Tuning systems beyond the standard twelve-tone frame, such as 24-, 31- or 96-tones per octave, provide composers with increased resources for musical colour, texture, harmony and expressive nuance. For the composer the consequent vast increase in data demands advanced organisational strategies, and new or adapted musical instruments. Despite attempts to systematise microtonality, we continue to lack codified methods for dealing with microtonal tuning constructs as holistic entities, beyond microtonal ‘inflections’ of what are otherwise twelve-note contexts. Recent demonstrations show that strictly formalised techniques of musical organisation offer potential solutions to the conceptualisation and handling of microtonal tunings but lack connections to intuitive pathways to employ them in composition. Emphasising the importance of blending systematic and intuitive approaches to composition, this research will devise and synthesise formalised generative systems through which the subtleties and complexities of microtonal tunings can be effectively handled and explored in composition to discover, compare and develop the expanded harmonic and melodic principles they afford.