Light rail transit (LRT) systems are vital aspects of the worldwide endeavor to achieve transport sustainability and have been essential in enhancing the economies of urban areas. Issues such as pollution, the risk of road accidents, and traffic congestion could be resolved using this progressive alternative. The statistics showed that only 20% of the commuters in Malaysia use public transport, including LRT, and 80% use private transportation. It is relatively low compared to other Asian countries. High-quality service is essential to improve users’ perceived satisfaction with the provided services and increase LRT ridership. The objective of the present study is to acquire an understanding of which factors are crucially influential on users’ perceptions of satisfaction. In-person questionnaires were utilized to obtain the information for this paper, with a total of 417 LRT riders in Malaysia’s Klang Valley surveyed. This study adopted the factor analysis, correlation test, and artificial neural network (ANN) model. Eight elements related to the quality of service were extracted to ascertain how they influenced the perceived satisfaction of users: information signs, ticket-based services, amenities, safety, employee performance, speed, comfort, and the service details available to riders. Each factor was significantly related to the perceptions of satisfaction, according to the correlation test. Finally, the ANN model shows that the dominant factors determining the LRT users’ perceived satisfaction are the signage, amenities, and provision of information. The findings of this research should benefit the providers of services, policy makers, and planning departments by enabling them to formulate successful approaches that ensure user satisfaction is enhanced and the number of riders on the LRT increases.