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This article addresses the urgent need to combat climate change by exploring Nature-based Solutions (NbS) for carbon capture, utilization, and storage (CCUS). The existing CCUS technologies face challenges of maturity, energy intensity, and high costs. To answer this challenge, this work proposes a new design methodology to facilitate the identification, evaluation and scaling of NbS for CCUS in a systematic and impactful manner. The proposed method involves analyzing a problem, identifying the required function, and using keywords to guide the research. Through iteration, the array of potential solutions expands, providing diverse options with various biological functions. Then, the focus shifts to narrowing down the most promising solutions to reduce the number of potential NbS. Common functions are identified, solutions are organized by domain, and priorities are set based on ability, effectiveness, and cost. Finally, scalability insights, as well as the enablers and barriers, are identified to design a roadmap for scaling the NbS. Applied to the case study of CCUS, 68 NbS emerged, including bivalve, and carbonic anhydrase for example. The method then narrowed down the research to five top solutions: cactus, mycorrhizal fungi, microalgae, cobalt oxide and rocks (basalt, olivine) for enhanced weathering. This approach facilitates the efficient identification of promising NbS. Subsequently, scalability insights and a roadmap were developed, using the example of the Opuntia ficus-indica cactus, which was one of the five NbS selected.