This paper presents a new method for forecasting cyclist volume and route choice based on space syntax techniques for urban analysis. Space syntax has been shown to correlate strongly with pedestrian and vehicular trips in a number of international studies, but little research to date has focused on the role of urban form and street network design in cyclist route choice. This paper addresses this gap by analyzing the distribution of cycling trips in the central London area, focusing on a sample of work-based commuting trips. A sample of 423 cyclists from 50 organizations was combined with cordon volume counts at several Central London locations. It was found that individual cycle trips were subject to a wide range of variables that made individual traces difficult to predict, but that total cyclist volumes corresponded strongly with the most accessible, direct streets in the urban network. This research suggests that angular minimization is an important factor in cyclist route choice and that measurement of least angle routes in urban environments can be a useful way of predicting cyclist volumes and route choice. Such techniques have the potential to save planners and policymakers the expense of performing origin destination studies and may offer a useful tool for cyclist volume prediction.