Public transportation in Phnom Penh, Cambodia has undergone significant changes in recent years, with daily ridership increasing from 7,000 at its reintroduction in 2014 to about 20,000 passengers by 2023. Despite this progress, a considerable portion of the buses operate at around 50% of their total capacity, presenting a challenge to the system’s efficiency and sustainability. In order to shift Phnom Penh towards a more sustainable transportation future, an examination of transit loyalty emerges as a strategy to retain and attract more users. This study aims to contribute to the understanding of urban public mobility in the context of a developing country, by investigating the relationships among accessibility, perceived value, satisfaction, service quality, and loyalty, as well as exploring the perceptions of loyal users of the public buses. Data collection was conducted through in-person and questionnaire-based interviews at bus stops and on the buses. Out of the 220 responses gathered, 186 were deemed suitable for further factor and reliability analyses. Finally, the data were analyzed using a Structural Equation Modelling (SEM) approach, and the best fitting model was developed to illustrate the relationship among the constructs of transit loyalty. Findings suggest that loyalty is primarily influenced by satisfaction, which is driven by perceived value and accessibility. Furthermore, service quality was found to have an impact on perceived value. This study suggests that there is a strong possibility for more demand for public transportation for non-bus users, provided the system offers better coverage and frequency. Consequently, this presents as an opportunity for policymakers and stakeholders to leverage these insights in shaping policies that would enhance the sustainability and appeal of public transportation in Phnom Penh.