Considerable interest has been shown in decreasing car use through planning and policy-making efforts. However, little is known about the interactive effects of built environment (BE) and parking policy on car use, and it is unclear whether and how these effects differ across trip purposes. We conducted a web-based survey in Beijing and collected data from 1036 respondents, including 517 male and 519 female respondents. This study estimates the interactive effects of BE and parking policy on car use for home-based work and non-work trips by employing multilevel logit models. The results show that BE variables at trip origins and destinations are important for shaping car use for both home-based work and non-work trips. Specifically, land use mixture (Coeff. = −0.121), bus stop density (Coeff. = −0.006), and population density (Coeff. = −0.009) at residential locations are negative factors affecting car use for work trips, whereas distance to local center (Coeff. = 0.012) and distance to the city center (Coeff. = 0.019) at residential locations are positive factors. Land use mixture (Coeff. = −0.323), bus stop density (Coeff. = −0.008), road density (Coeff. = −0.002), and population density (Coeff. = −0.007) at residential locations are negative factors of car use for non-work trips. Among BE factors at destinations, land use mixture (Coeff. = −0.319), bus stop density (Coeff. = −0.015), road density (Coeff. = −0.008), distance to the local center (Coeff. = −0.018), and population density (Coeff. = −0.012) are negative factors for car use for work trips, whereas the negative factors for non-work trips are land use mix (Coeff. = −0. 218), bus stop density (Coeff. = −0.038), road density (Coeff. = −0.003), distance to the city center (Coeff. = −0.121), and population density (Coeff. = −0.009). The effects of BE variables can be strengthened or weakened by free parking and parking convenience. Moreover, the results identify significant differences in the effects between work and non-work trips. These findings inform planners and policymakers of how to coordinate the BE and parking policies to decrease car dependence.