In nature, Tessellated Material Systems (TMS) appear convergently across species and at all length scales. Their evolutionary success is based on the ability to unify mechanically opposing properties in one functional system. While the application of tessellations in Design and Architecture was and is focusing on the geometrical and structural benefits, this practice-based PhD project explores a different Design approach shifting the focus from structure to material. The aim of this research is to develop methods for designing hierarchical materials that lead to multi-functionality allowing for context sensitivity.