Topological interlocking assembly (TIA) and computational architecture treat form as an emergent property of a material system, where the final shape results from the interplay of geometries and geometric interdependencies influenced by material, structural, and fabrication constraints. This paper posits that TIA is an ideal pedagogical tool for introducing students to computational architecture, its theoretical foundations and design principles. Specifically, defining TIA as a material system provides a robust educational approach for engaging students with computation, fostering design processes through bottom-up, hands-on investigations and procedural logic, understanding generative geometric rules, and exploring the flexibility of parametric variations. The methodology is illustrated through a Design Workshop and study unit from the Bachelor’s and Master’s programs at the Faculty for the Built Environment, University of Malta. The paper presents four investigations of defining a material system based on TIA - of tetrahedra, cones, octahedra, and osteomorphic blocks—as case studies to demonstrate how these exercises introduce students to computational thinking, parametric design, and fabrication techniques. Finally, the paper discusses the advantages and limitations of this pedagogical methodology.