This study outlines the development of clay and ceramic-based living biocomposite materials under minimal moisture environments. The biocomposites supported live and metabolically active photosynthetic microorganisms (microalgae). The work sets out laboratory testing strategies to assess the limiting conditions for life within living materials to inform the conditions needed for sustained operation. Combinations of clay/ceramic-based substrate types, nutrient loadings, amounts of moisture exposures, and operation times were explored. As a result, microalgae (Chlorella vulgaris) colonized both clay and ceramic forms, showing operational longevity of 100 days, even with low nutrient exposure. Further iterations of these sustainable living materials may prove useful for local potential carbon dioxide removal to improve air quality and reduce the carbon footprint and operation costs of mechanically ventilated spaces. © 2020 Association of Collegiate Schools of Architecture.