Sustainability is increasingly recognized as a key innovation capability in the organization. However, it is not always evident for manufacturers how sustainability targets shall be “mixed and matched” with more traditional objectives—such as quality, time, cost, and performances—when designing and developing solutions. The emergence of “servitization” and product-service systems (PSS) further emphasizes the need for making thoughtful trade-offs between technical aspects, business strategies, and environmental benefits of a design. The objective of this paper is to investigate how multi-criteria decision making (MCDM) models shall be applied to down-select PSS concepts from a value perspective, by considering sustainability as one of the attributes of a design contributing to the overall value of a solution. Emerging from the findings of a multiple case study in the aerospace and construction sector, the paper presents a five-step iterative process to support decision making for sustainable PSS design, which was further applied to design an electrical load carrier. The findings show that the proposed approach creates a “hub” where argumentations related to “value” and “sustainability” of PSS solution concepts can be systematically captured in a way that supports the discussion on the appropriate quantification strategy.