This paper describes an adaptive decision-making design framework for investigating the synergies between aesthetically-driven and performance-driven criteria, specifically in designing the material behaviour of an electroresponsive building envelope system. An immersive and interactive simulation environment developed in the C++ programming language provides a computational tool for testing the visual and energetic performance of a dynamic building envelope as it negotiates bioclimatic energy flows with participants’ aesthetic preferences and interactions. Experiments in bioresponsive feedback loops examine the impacts that user engagement and real-time energy performance feedback have on participants’ design choices. Preliminary results demonstrate that exposure to energy performance feedback and to the collective design choices of multiple users leads to adaptive decision-making that favours synergistic system performance with the potential for increased socio-ecological connections. Critically, this research provides new methods for supporting the design of emerging material behaviours for dynamic building envelopes that can negotiate multiple performance criteria.