Chemical stimulation sustains bioluminescence of living light materials.

Bioluminescence offers a powerful tool for real-time, label-free sensing for living materials. However, conventional approaches often rely on mechanical stimulation, which is difficult to standardize, localize, and sustain. Here, we introduce a chemical strategy to stimulate and sustain bioluminescence in the marine dinoflagellate Pyrocystis lunula, enabling durable, adaptive, light-emitting living materials. By embedding P. lunula into 3D-printed, alginate scaffolds, we engineered architecturally stable constructs with long-term cellular retention, viability, and light-emitting capacity. Exposure to acidic and basic environments produced chemically encoded bioluminescent signatures: Acid triggered localized, persistent emission, while base induced diffuse, biphasic emission indicative of cellular stress. Notably, combining chemical and mechanical stimulation led to enhanced total bioluminescence emission, achieving greater amplitude and duration of light emission without compromising cell mechanoresponsiveness. Longitudinal studies over 4 weeks demonstrated that our materials retain responsiveness and structural integrity across repeated stimulation cycles, overcoming single-use limitations. Together, these findings establish a chemistry-controlled platform for light-emitting living materials for biosensing, soft robotics, and environmental monitoring.