Residents are significantly affected by air pollution during their travels. When air pollution increases, they may opt for zero-pollution travel to improve air quality. This study uses dual fixed effects, mediation effects, and geographically weighted negative binomial regression models to analyze the impact of transportation-induced air pollution on residents’ zero-pollution travel. Data from 33 administrative districts in London (2018–2022) include transportation-related air pollutants, Google Trends on “Air pollution” and “Transportation,” and residents’ willingness to travel zero-pollution. Results show a positive correlation between mainstream air pollutants and residents’ willingness to travel zero-pollution, with concerns about air pollution mediating this relationship. In terms of travel modes, residents’ willingness to cycle is highly sensitive to air pollutants, especially NOX, while walking shows partial sensitivity. The study also finds that NOX has the strongest impact on residents’ willingness to travel with zero pollution. During the COVID-19 pandemic, changes in travel behavior were observed: the willingness to bike decreased in sensitivity to most pollutants, while walking sensitivity increased. This indicates that health concerns during the pandemic influenced travel choices, with more residents opting for walking to reduce exposure to polluted environments. The research highlights the importance of addressing transportation-induced air pollution to encourage zero-pollution travel and improve urban air quality. By focusing on specific pollutants and residents’ concerns, policies can be tailored to enhance sustainable travel behaviors and reduce overall pollution levels. This study contributes to a better understanding of the dynamic relationship between air pollution and travel behavior, offering valuable insights for urban planning and public health strategies. It underscores the need for comprehensive measures to mitigate air pollution and promote healthier, zero-pollution travel options for residents, ultimately leading to more sustainable and livable urban environments.