ABSTRACT In this study, silicon‐based hybrid material modifiers were synthesized using organic–inorganic hybridization methods from polyvinyl alcohol and nano‐SiO 2 as principal raw materials. The effects of the hybridization ratio and various factors on the workability and mechanical properties of cement mortar were systematically studied. Subsequently, the hybrid material modifiers were optimized to improve cement performance to enhance recycled aggregate. The experimental results show that the hybrid enhancement with the developed silicon‐based modifiers improved mortar workability, increased its water retention, and reduced the water absorption rate of recycled aggregate by 35%, in addition to a 30% decrease in the crushing value.