Accessibility of travel may be better understood if psychological factors underlying change in travel behavior are known. This paper examines older (65+) travelers’ motives for changing their travel behavior. These changes are grounded in critical incidents earlier encountered in public-transport travel. A scientific framework is developed based on cognitive and behavioral theory. In 29 individual interviews, travelers’ critical reactions (i.e., cognitive, emotional, and/or behavioral) to 77 critical incidents were examined. By applying critical incident technique (CIT), five reaction themes were identified that had generated travel-behavior change: firm restrictions, unpredictability, unfair treatment, complicated trips, and earlier adverse experiences. To improve older travelers’ access to public transport, key findings were: (a) service must be designed so as to strengthen the feeling of being in control throughout the journey; (b) extended personal service would increase predictability in the travel chain and decrease travel complexity; consequently, (c) when designing new services and making effective accessibility interventions, policy makers should consider and utilize underlying psychological factors that could direct traveler behavior.