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Urban spatial structure is a critical component of urban planning and development, and among the different urban spatial structure strategies, ‘polycentric mega-city region (PMR)’ has recently received great research and public policy interest in China. However, there is a lack of systematic understanding on the spatiality of PMR from a pluralistic perspective. This study aims to fill this gap by investigating the spatiality of PMR in the Yangtze River Delta Urban Agglomeration (YRDUA) using city-level data on gross domestic product (GDP), population share, and urban income growth for the period 2000–2013. The results reveal that economically, the YRDUA is experiencing greater polycentricity, but in terms of social welfare, the region manifests growing monocentricity. We further find that the triple transition framework (marketization, urbanization, and decentralization) can greatly explain the observed patterns. Although the economic goals are accomplished with better spatial linkages and early economic development policies, inequality in spatial distribution of public services and the continuing legacy of central planning remain barriers for the YRDUA to emerge as a successful PMR. The results of this research offer meaningful insights on the impact of polycentric policies in the YRDUA and support policymakers in the implementation of appropriate urban spatial development strategies.