The sustainable development of urban transport is the key to sustainable urban development. This study analyses and identifies the evaluation indicators affecting Macau’s transport, and analyses the relationship between the relevant evaluation indicators and passenger satisfaction, thus contributing to the improvement and the sustainable development of Macau’s public transport services. This study uses a questionnaire to collect data. Based on the current situation of Macau’s social groups, the mainland students in Macau who were selected as the target group are significantly different from residents and tourists in Macau; their needs and perceptions of public transport are more intense. This group’s needs and perceptions of public transport are significantly different from those of residents and tourists. The set indicators of satisfaction with public transport in Macau reflect them. After analyzing and determining the evaluation indicators, structural equation modeling was applied to establish the structural models of Macau’s three public transport services. Finally, the shortcomings of the three public transport services were reflected through the standardized coefficient weights and passenger satisfaction. The study results show that the seating arrangement and smoothness of travel of Macau’s public transport services need to be improved, and the dial-a-ride service’s price setting and waiting time need to be improved. The price setting, convenience of hailing, and payment method of the taxi service need to be improved. In contrast, overall, the satisfaction level of the dial-a-ride service is significantly higher than that of the taxi service. Therefore, the findings of the study have important policy implications for relevant policymakers, who should not only focus on optimizing daily operations but, more importantly, on improving the shortcomings mentioned above, which are of great value in enhancing the passengers’ perception of public transport in Macau and are also crucial to achieving the sustainable development of public transport in Macau.