Transit-oriented development (TOD) is an established urban planning principle for increasing public transport (PT) use. However, whether TOD enhances perceived safety and increases PT use remains an open question. This study analyzes the link between mode choice, perceived safety, and TOD dimensions on a large dataset covering the Greater Copenhagen area in Denmark. Using survey data and site observations, we first estimate multiple linear regression models to show which TOD dimensions enhance individuals' perceived safety at train stations. Then, using large-scale travel survey data encompassing 21,844 trips between 2009 and 2018, including various user socioeconomic variables, we estimate a mode choice model in which TOD score and perceived safety are used as explanatory variables. Our results provide empirical evidence showing that the safety dimension of TOD significantly increases perceived safety and that perceived safety at both the home and activity ends of the trip influences the likelihood of an individual choosing PT. Only a higher TOD score at the activity end significantly increases PT use, whereas park-and-ride lots at the activity end reduce it and make cycling less attractive at both trip ends. Distance to the nearest stations/stops and service headway have a significant influence on mode choice at both ends of the trip. These results indicate that dense urban development around stations supports PT use and cycling more strongly than allocating space to park-and-ride lots. Our results are important for policymakers seeking to use TOD guidelines to increase individuals' perceived safety and PT use in cities.