Driven by technological progress and market demand, the optimization and adjustment of grain planting structure played an important role in increasing grain output. Due to the great difference between the yield per unit area of different types of food crops, the consumption of cropland and water resources has a significant change during the grain growth. From the perspective of structural adjustment, rather than the usual productive factor input, we analyze the process of adjustment for grain planting structure in China and its effect on the consumption of cropland and water resources by using the scenario comparative analysis method. The results show that: (1) From 2003 to 2019, China’s grain output has increased steadily and the planting structure has changed greatly. Rice was replaced by corn to become the grain crop with the maximum proportion of planting area since 2007. The increase of corn planting structure proportion is concentrated in the northern regions. (2) At the national level, according to the adjustment of grain planting structure, the saving of cropland and water resources consumption showed a “cumulative effect” as time went on. (3) The saving effects of structural adjustment in the northern regions on cropland and water resources consumption are better than that in the southern regions, such as Northeast China Plain, Northern arid and semiarid region and Loess Plateau. (4) In reality, although the adjustment of grain planting structure saved lots of cropland and water resources, the continuous growth of grain output has increased the pressure on the ecological environment in the northern regions according to theirs water limits. Therefore, it is necessary to continuously optimize the grain planting structure and restrict land reclamation in northern China. In addition, to ensure food security, it is feasible to encourage the southern regions with abundant water and heat resources to increase the grain planting area and meet its self-sufficiency in grain demand.