Since the start of the new century, the focus of China’s socioeconomic development has gradually shifted from prioritizing efficiency to social equity, which is an important ingredient of sustainable development. The accessibility of public service facilities (PSFs) is vital for achieving social–spatial sustainability. As a basic tool for arranging PSFs, however, traditional urban plannings mainly focus on the spatial uniform distribution of facilities rather than the variance of the spatial distribution of populations they serve. So, by taking the dual perspective view, this paper quantitatively measures the balance of PSFs’ spatial distribution of and populations of Urumqi City at the sub-district level. Based on point of interest (POI) data, this paper calculates and analyzes Gini coefficients and location entropy of three basic PSF types: living service facilities (LSFs), primary schools and kindergartens (PSAKs), and medical facilities (MFs). The research finds that the Gini coefficients of LSFs, PSAKs, and MFs in Urumqi City are 0.42, 0.36, and 0.34, respectively. Moreover, there are three significant mismatch areas: an extremely high PSF index value in low-population sub-districts, an extremely low index value in remote suburbs, and an extremely low index value in the city center. These findings indicate an obvious imbalance between the spatial distribution of PSFs and the population in Urumqi, which may be a critical impediment to sustainable development. Based on these, this paper offers guidance for achieving sustainability in the allocation of spatial resources.