Grain production is inseparable from the support of water and land resources. The coordinated development of agricultural water and land resources is an important prerequisite to the sustainability and stability of national food security. From the angle of virtual water and cultivated land, this paper constructs the evaluation index system of the coordinated development of virtual water-virtual cultivated land composite system. With the adoption of coupling degree function and coupling coordination function, the coupling degree, coupling coordination degree and the evaluation of sub-system integrated development in 31 provinces of China in 1998, 2005, 2010 and 2017 were calculated and the development status of provincial virtual water-virtual cultivated land composite system of major grain crops in China was analyzed using time series and spatial autocorrelation method. The results show that the trends of the comprehensive development of the provincial virtual water systems and cultivated land systems were consistent, showing a process of decreasing-increasing-decreasing. Their spatial distribution pattern was high in the east and middle region but low in the west region, and the spatial differentiation was enhanced. In terms of coupling coordination and time series evolution, the provincial virtual water-virtual cultivated land composite systems of major grain crops had high coupling degree, water and land of the systems interacted with each other and formed a coupling symbiosis system; however, the coupling coordination degree of the composite systems was much lower than that of the coupling degree, which needs to be improved significantly. The hierarchical distribution structure was spindle-typed with "less at the ends but more in the middle". In spatial distribution, the provincial composite systems showed a significant positive spatial autocorrelation, but the spatial agglomeration types of most provinces were in an unstable state.