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The emerging population has increased travel demand and improved public transport mode in cities to connect the people. (1) Background: This study used the Theory of Planned Behavior (TPB) to assess the usage behavior for city rail transport with the factors attitude, subjective norm, and perceived behavioral control and its impact on pro-behavioral intentions to increase the actual usage of rail transports, i.e., LRT, MRT, and KTM commuter. (2) Method/Approach: To understand the antecedents of pro-environment behavioral intention, this study performed pilot testing, for which we collected the data through closed-ended questionnaires to test the instrument’s reliability, specifically from the Klang Valley in Malaysia. (3) Findings/Results: This study revealed that the public attitude due to environmental concern and subjective norms and perceived behavioral control are the strongest predictors for public transport usage through behavioral intention. The study estimated that most respondents would have agreed to choose public transport mode if quality of services increased. (4) Conclusion: In future research, the goal of this study could be extended as a strategic indicator for sustainable development through efficient mobility choice in Malaysia. The TPB model helps to present the factors involved in growing and retaining clients for rail transport. In terms of implications for policy, this study also provides policymakers with valuable information to maintain the current public transport passengers and attract new users through the perceived service quality and customer satisfaction of public transport.