Population mobility patterns are an important reflection of the future distribution of migrant populations and the evolution trends of urbanization patterns. However, although research based on statistical data can reveal the pattern of population flow, it also shows a time lag. Most of the population flow network research based on location services data has failed to fully discuss the symmetry of directional outflows and inflows in the same place and the two-way symmetrical connections between places. This paper creatively proposes and constructs the concept and analysis framework of population flow asymmetry. We used the Yangtze River Delta (YRD) as a typical case and the results of our analysis reveal the temporal and spatial asymmetry of the population flow using complex network analysis methods based on the Spring Festival (SF) population migration big data. We found that the timing asymmetry manifested in such a way that the closer it was to the festival, the greater the scale and intensity of the population movement. This is a feature of the lack of scale and regional differences within China. The spatial asymmetry was manifested in three aspects, network, node, and link, and the core cities with administrative and economic hierarchical advantages dominated the asymmetric pattern of regional population mobility. In addition, distance and administrative boundaries are factors that cannot be ignored in population movements, and they were implicated in the degree of asymmetry by distance enhancement and administrative boundary blocking. The conclusions of this study can not only provide policy decision-making guidelines for population management and resource allocation in the YRD, but they can also provide a reference value for achieving the goal of regional, high-quality, integrated development. Future research will further the discussion and management of socio-economic attributes in order to develop a more detailed and microscopic understanding of the mechanisms of population mobility patterns.