Cyber–physical–social systems (CPSS) with highly integrated functions of sensing, actuation, computation, and communication are becoming the mainstream consumer and commercial products. The performance of CPSS heavily relies on the information sharing between devices. Given the extensive data collection and sharing, security and privacy are of major concerns. Thus, one major challenge of designing those CPSS is how to incorporate the perception of trust in product and systems design. Recently, a trust quantification method was proposed to measure the trustworthiness of CPSS by quantitative metrics of ability, benevolence, and integrity. The CPSS network architecture can be optimized by choosing a subnet such that the trust metrics are maximized. The combinatorial network optimization problem, however, is computationally challenging. Most of the available global optimization algorithms for solving such problems are heuristic methods. In this paper, a surrogate-based discrete Bayesian optimization method is developed to perform network design, where the most trustworthy CPSS network with respect to a reference node is formed to collaborate and share information with. The applications of ability and benevolence metrics in design optimization of CPSS architecture are demonstrated.