Amid ongoing advancements in the transportation sector, the commercial viability of electric Vertical Take-Off and Landing (eVTOL) vehicles is being evaluated for their potential to offer flexible, reliable, rapid, and eco-friendly mobility solutions. While the engineering aspects of eVTOL vehicles have been extensively studied worldwide, the sustainable adoption of this technology has not yet been fully explored. To bridge this gap, the current study first identifies sustainable adoption strategies for eVTOL vehicles in shared passenger and freight transportation arrangements and then evaluates them using the Grey-DEMATEL (Decision-Making Trial and Evaluation Laboratory) method. The methodology uncovers the causal relationships between these strategies and highlights their criticality, allowing for the prioritization of the most essential ones. The key contribution of this study lies in emphasizing top-ranked strategies, particularly the enhancement of customer adoption, which is often overlooked in the existing literature. Most published studies focus primarily on the technical aspects of this innovation, neglecting the crucial importance of prioritizing customer acceptance for sustainable adoption. Additionally, we identified that government support, financial incentives such as subsidies, and a strong understanding of the technology are critical focus areas for accelerating adoption. This study makes a significant contribution by being one of the first attempts to create a Grey-DEMATEL-based framework for evaluating sustainable adoption strategies in the context of eVTOL vehicles’ deployment in shared passenger and freight transportation arrangements. Lastly, a sensitivity analysis is conducted to ensure the robustness of the method; consequently, the entire framework is found to be robust.