The transition to low-carbon mobility has emerged as a key objective of climate action. While much is known about the determinants of modal shifts between cars and other modes, little research was conducted on the dynamic relationships between working from home (WFH), commute distance, mode preference, and car use. Applying random intercept cross-lagged panel modeling, this study provides a six-year (2017–2022) longitudinal analysis in the Netherlands to investigate the bidirectional effects among these targeted variables while accounting for the effects of built environment attributes and life events. Results show that WFH was associated with a significant reduction in car use frequency and higher levels of WFH were related to longer commute distance during COVID-19, while a preference for cars was linked to sustained car use in general. We also found significant effects of urbanity, land use diversity, distance to public transit, and intersection density on car use, car preference, and WFH. In addition, life events, such as job changes, childbirth, and relocation, played a role in reshaping mobility and work behaviors. Therefore, the important roles of WFH, commute distances, mode preference, built environment, and life events provide great implications for transitioning to low-carbon mobility.