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 contextual constraints (material, structure, and fabrication). This paper posits that TIA is an ideal pedagogical tool for introducing students to computational architecture, and 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; expressing design intents as procedural logic; understanding generative geometric rules; and exploring the flexibility of parametric variations. The methodology is detailed and 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. Four case studies of TIA—of tetrahedra, cones, octahedra, and osteomorphic blocks—demonstrate how these exercises introduce students to computational thinking, parametric design, and fabrication techniques. This paper discusses the advantages and limitations of this pedagogical methodology, concluding that integrating computational architecture in education shifts students’ design processes to investigation and innovation-based approaches, enabling them to address contemporary design challenges through context-driven solutions.