Hempcrete is a sustainable biocomposite that can reduce buildings’ embodied energy while improving energy performance and indoor environmental quality. This research aims to develop novel insulating hemp-lime composites using innovative binder mixes made of recycled and low-embodied energy pozzolans. The characterization of composites’ mechanical and hygrothermal properties includes measuring compressive strength, splitting tensile strength, thermal conductivity, specific heat capacity, and moisture buffer capacities. This study also investigates the impact of sample densities and water content on compressive strength at different ages. The findings suggest that mixes with a 1:1 binder to hemp ratio and 300−400 kg/m³ density have hygrothermal and mechanical properties suitable for insulating infill wall applications. Hence, compressive strengths, thermal conductivity, and specific heat capacity values range from 0.09 to 0.57 MPa, 0.087 to 0.10 W/m K, and 1250 to 1557 J/kg K, respectively. The average moisture buffer value for all hempcrete samples of 2.78 (gm/m² RH%) indicates excellent moisture buffering capacity. Recycled crushed brick pozzolan can enhance the hygrothermal performance of the hemp-lime composites. Thus, samples with 10% crushed brick have the lowest thermal conductivity considering their density and the highest moisture buffer capacity. The new formulas of hydrated lime and crushed brick have mechanical properties comparable to metakaolin and hydraulic lime formulas.

Phase change material (PCM)-enhanced building envelopes can control indoor temperatures and save energy. However, PCM needs to undergo a phase change transition from solid to liquid and back to be fully effective. Furthermore, most previous research integrated PCM with high embodied energy materials. This study aims to advance the existing research on integrating PCM into carbon-negative wall assemblies composed of hempcrete and applying temperature control strategies to improve wall systems’ performance while considering the hysteresis phenomenon. Four hempcrete and hempcrete-PCM (HPCM) wall design configurations were simulated and compared under different control strategies designed to reduce energy demand while enhancing the phase change transition of the microencapsulated PCM. The HPCM wall types outperformed the hempcrete wall assembly through heating (~3–7%) and cooling (~7.8–20.7%) energy savings. HPCM walls also maintained higher wall surface temperatures during the coldest days, lower during the warmest days, and within a tighter range than hempcrete assembly, thus improving the thermal comfort. However, the results also show that the optimal performance of thermal energy storage materials requires temperature controls that facilitate their charge and discharge. Hence, applied control strategies reduced heating and cooling energy demand in the range of ~4.4–21.5% and ~14.5–55%, respectively.