Controllable reciprocating seal (CRS) is a new generation of intelligent seal with performance regulation function, but its high-performance design optimization method remains unclear, which is an important issue that determines its entire life cycle. To address it, this paper takes hydraulically controllable reciprocating seals (HCRS) as the research object, and employs a mixed thermoelastohydrodynamic lubrication (TEHL) model to establish a structure-material multi-objective co-design optimization model that integrates static and dynamic sealing performance. The optimal combination of sealing structure and material parameters is obtained with the objective functions of minimizing the maximum von Mises stress, net leakage, and frictional power loss. By comparing the static and dynamic sealing performance of seals under three methods of single structural design optimization, single material design optimization, and structure-material collaborative optimization under each optimal parameters, the superiority of the collaborative design optimization method proposed in this paper has been demonstrated. Compared with single structural or material optimization methods, its maximum von Mises stress, net leakage, and frictional power loss have been improved by 66.81%, 21.73%, and 43.67%, respectively. Therefore, the collaborative design optimization of structural and material parameters is a more efficient optimization design method and is recommended for engineering applications.