Smart product service system (PSS) has become an essential strategy to transform towards digital servitization for manufacturing companies. By leveraging smart capabilities, smart PSS aims to create superior user experience in a smart context. To develop a successful smart PSS, customer requirement management from smart experience perspective is necessary. However, it is a challenging task to identify and evaluate diverse, implicit and interrelated smart experience-oriented customer requirement (SEO-CR) in smart PSS context. Hence, this paper proposes an effective methodology to elicit and analyze SEO-CRs. At first, a generic, two-dimensional SEO-CR system is presented as a basis to derive the tailored SEO-CRs for various smart PSS applications. Second, a novel HFLC-DEMATEL (hesitant fuzzy linguistic cloud-based Decision-making and trial evaluation laboratory) method is proposed to accurately evaluate the priority and complicated interaction of SEO-CRs, considering the hesitancy, fuzziness and randomness under uncertain decision environment. Some new operations (e.g., cloud total-relation matrix and weight determination method) and a cloud influence relation map are developed to fully take advantage of cloud model in DEMATEL implementation. Finally, a real case of smart vehicle service system (SVSS) is presented. The 18 SEO-CRs of the SVSS are derived based on the generalized SEO-CRs. By using HFLC-DEMATEL, some important SEO-CRs in context of SVSS are identified, such as autonomous and convenience. The finding of results can help designers make proper decisions in design and development of SVSS with a superior smart experience. The effectiveness and reliability of the proposed method are validated by conducting some comparative analyses.