Despite extensive regulations, the systemic under-reporting of construction and demolition waste generation rates pervades the South African waste sector due to the extensive and active informal waste management practices that are typical of developing countries. This study merges the rapid development of high-technology 3D-printed concrete (3DPC) with the increasing pressure that the built environment is placing on both natural resource consumption and landfill space due to construction and demolition waste (CDW) by establishing an inventory of CDW that is suitable for use in 3DPC in South Africa. This is an essential step in ensuring the technical, economic, and logistical viability of using CDW as aggregate or supplementary cementitious materials in 3DPC. Of the methods considered, the lifetime material analysis and per capita multiplier methods are the most appropriate for the context and available seed data; this results in CDW estimates of 24.3 Mt and 12.2 Mt per annum in South Africa, respectively. This range is due to the different points of estimation for the two methods considered, and the per capita multiplier method provides an inevitable underestimation. In order to contextualise the estimated availability of CDW material for use in concrete in general, the demand for coarse and fine aggregate and supplementary cementitious material in South Africa is quantified as 77.9 Mt. This overall annual demand far exceeds the estimated CDW material (12.2–24.3 Mt) available as an alternative material source for concrete.