Mobile devices for city-scale air quality monitoring is receiving increasing attention due to the advent of low-cost and miniaturized sensors. Mobility and crowdsensing have emerged as a new means to investigate the ambient air quality in urban areas. However, the design of the network (e.g., number of sensors per unit area) and the scientific interpretation of collected data with an ad hoc method are still challenging. In this paper, we focus on the use of a fleet of private bicycles to monitor NO 2 concentrations in the city of Marseille, France. The study is based on synthetic observations generated by means of a regional air quality simulation system at a spatial resolution of 25 m × 25 m and simulated bike trips that are randomly generated in the city. The bike trips correspond to a maximum of 4500 bike commuters and are generated using a web-based navigation service. Simulated bike tracks are validated using available statistics on bike counts. Each bike track is associated with the along-track corresponding NO 2 concentrations collected from the air quality simulations and physical features on the ground collected from Open Street Map. Spatialization of the information collected aboard the bikes is tested by using three different algorithms: kriging, land-use regression (LUR) and neural network (NN). LUR and NN show that the fleet can be limited to below 100 bikes while the performance of kriging is steadily increasing with the number of bikes. Increasing the sample distance above 200 m also impairs the citywide prediction of simulated NO 2 concentrations.