As computational design processes have moved from representation to simulation, the focus has shifted towards advanced integration of performance as a form defining measure. Performance, though, is often assessed purely on the level of geometry and stratified between hierarchically independent layers. When looking at tension-active membrane systems, performance is integrated across multiple levels and with only the membrane material itself, defining the structural, spatial and atmospheric qualities. The research described in this paper investigates the integrative nature of this type of lightweight structure and proposes methodologies for generating highly articulated and differentiated systems. As material is a critical component, the research focuses on a system-based approach which places priority on the inclusion of material research and parameterization into a behavior-based computational process.