Lightweight porous composites have been widely explored to improve their acoustic and thermal performances. Hempcrete can serve as thermal insulating or soundproofing material by utilising its high porosity. However, the rigorous correlation between hempcrete thermal and acoustic performance and its pore structure remains poorly understood due to its different pore types. In this study, three hempcrete pore types [i.e., i) inter-pore between hemp and mortar, ii) hemp intra-pore, and iii) mortar intra-pore] were modified by tamping, delignification, and foaming agent conditions, respectively. Then the volumes of three types of pores were estimated using X-ray micro-computed tomography (μCT) and mercury intrusion porosimetry. The new segmentation methods were developed and their reliability and accuracy were validated. Then, the pore volumes were correlated to the thermal and acoustic properties of hempcrete. Low tamping and high delignification conditions are recommended to increase inter-pore volume and enhance hempcrete performances relating to both thermal insulation and sound absorption for real-world hempcrete applications.