Plastics represent an integral part of our everyday lives, with various functions from packaging materials to insulation layers in our buildings. Pure expanded polystyrene (EPS) is a good example of a fully recyclable material. However, once polluted with other materials or substances, EPS becomes a serious environmental burden. In this work, waste EPS for the production of greener building composites with balanced properties and utility value was investigated. Natural aggregate (2/4 mm) was substituted with corresponding fractions of a thermoplastic alternative in portions of 25, 50, 75, and 100 vol.%. The comprehensive experimental investigation evaluated physical and mechanical properties, heat transport and accumulation, and water absorption characteristics. Due to the uniformly distributed plastic particles in the hardened cement-based matrix, the data revealed an important reduction in the dead weight of produced mortars, which also reduced thermal conductivity by up to 47%. On one hand, lightweight mortars showed partially reduced mechanical resistivity; on the other hand, the EPS bead-modified structure turned out to be effective in liquid water transport reduction.