Harnessing the symbiotic association of plant and fungi, we devised SimbioBrick; a living system that encases mycorrhizal fungi and alfalfa in a portable pot-like brick cassette that promotes plant growth and carbon sequestration. SimbioBrick contains fungal spores, seeds, water, and nutrient-storing hydrogels emulating wet soils. Their outer geometries are designed to provide structural support in modular assemblies and to expose plants to sunlight for photosynthesis. Their inner structures mediate depth for fungal colonization and porosity for adequate drainage. The SimbioBrick system is multifunctional in providing (1) biological behavior driven modular brick design, (2) indoor and outdoor oxygen production, (3) continuous carbon sequestration, (4) retaining water to self-irrigate, as well as (5) soil-bioremediation in our future work. Applications of the SimbioBrick system are living building components supporting bio-receptive architecture, such as substitution of heavy, multi-material, energy intensive, and non-recyclable green facades, or production of new outdoor flooring able to pave walkways while offsetting carbon emission from buildings and bio-remediating polluted soils beneath.