Cycling as a mode of transportation brings certain benefits to the user, such as improving health and saving money. It can provide a significant improvement in the quality of city life with minimal ecological impact. Thus, public bike-sharing systems have been adopted as a modal choice in many cities world-wide. However, there are some problems that must be addressed when designing a bike-sharing system, one of which is how to improve service quality and attract more users. This study proposes a hybrid model, combining the Decision-Making Trial and Evaluation Laboratory (DEMATAL) method with the Analytical Network Process (ANP) approach (called DANP), which addresses the dependent relationships between the various criteria for the quality of service for bike-sharing systems to better reflect the real-world situation. After building a complex evaluation system, a modified VIKOR (VlseKriterijumska Optimizacija I Kompromisno Resenje) method is applied to explore the weighted-gap to the aspiration levels. Furthermore, given the vagaries of human judgments and ratings, preferences cannot be assigned an exact numerical value, which can make it difficult to evaluate the performance or make comparisons. One way to improve upon this uncertainty is to apply Grey Theory. The proposed method is then applied using data for Taipei's Youbike and Obike systems. The analytical results and the resultant managerial applications for improving the service quality of both bike-sharing systems are also discussed with particular attention to the current policies of Taipei City.