Existing urban boundaries are usually defined by government agencies for administrative, economic, and political purposes. Defining urban boundaries that consider socio-economic relationships and citizen commute patterns is important for many aspects of urban and regional planning. In this paper, we describe a method to delineate urban boundaries based upon human interactions with physical space inferred from social media. Specifically, we depicted the urban boundaries of Great Britain using a mobility network of Twitter user spatial interactions, which was inferred from over 69 million geo-located tweets. We define the non-administrative anthropographic boundaries in a hierarchical fashion based on different physical movement ranges of users derived from the collective mobility patterns of Twitter users in Great Britain. The results of strongly connected urban regions in the form of communities in the network space yield geographically cohesive, non-overlapping urban areas, which provide a clear delineation of the non-administrative anthropographic urban boundaries of Great Britain. The method was applied to both national (Great Britain) and municipal scales (the London metropolis). While our results corresponded well with the administrative boundaries, many unexpected and interesting boundaries were identified. Importantly, as the depicted urban boundaries exhibited a strong instance of spatial proximity, we employed a gravity model to understand the distance decay effects in shaping the delineated urban boundaries. The model explains how geographical distances found in the mobility patterns affect the interaction intensity among different non-administrative anthropographic urban areas, which provides new insights into human spatial interactions with urban space.