Transportation networks, from bicycle paths to buses and railways, are the backbone of urban mobility. In large metropolitan areas, the integration of different transport modes has become crucial to guarantee the fast and sustainable flow of people. Using a network science approach, multimodal transport systems can be described as multilayer networks, where the networks associated to different transport modes are not considered in isolation, but as a set of inter- connected layers. Despite the importance of multimodality in modern cities, a unified view of the topic is currently missing. Here, we provide a comprehensive overview of the emerging research areas of multilayer transport networks and multimodal urban mobility, focusing on contributions from the interdisciplinary fields of complex systems, urban data science, and science of cities. First, we present an introduction to the mathematical framework of multilayer networks. We apply it to survey models of multimodal infrastructures, as well as measures used for quantifying multimodality, and related empirical findings. We review modeling approaches and observational evidence in multimodal mobility and public transport system dynamics, focusing on integrated real-world mobility patterns, where individuals navigate urban systems using different transport modes. We then provide a survey of freely available datasets on multimodal infrastructure and mobility, and a list of open-source tools for their analyses. Finally, we conclude with an outlook on open research questions and promising directions for future research.