The Mid-eastern Inner Mongolia of China, a typical agro-pastoral transitional zone, has undergone rapid agricultural land use changes including land reclamation and cropland abandonment in past decades due to growing population and food demand, climatic variability, and land use policy such as the "Grain for Green" Project (GFG Project). It is significant to the regional ecology and sustainability to examine the pattern and its rationality of land use change. The processes of land reclamation and cropland abandonment were accessed by using land use change dataset for four periods of 1990, 1995, 2000, and 2005, derived from the interpretation of Landsat TM images. And then the rationality of land reclamation and cropland abandonment was analyzed based on the habitat suitability for cultivation. The results indicated that: (1) land reclamation was the dominant form of agricultural land use change from 1990 to 2005, the total cropland area increased from 64,954.64 km(2) in 1990 to 76,258.51 km(2) in 2005; However, the speed of land reclamation decreased while cropland abandonment increased around 2000. The Land Reclamation Degree decreased from 1995-2000 to 2000-2005, meanwhile, Cropland Abandonment Degree increased. (2) As for the habitat suitability levels, moderately and marginally suitable levels had largest areas where cropland was widespread. Pattern of agricultural land use trended to become more rational due to the decrease of land reclamation area in low suitable levels and the increase of cropland abandonment in unsuitable area after 2000. (3) The habitat suitability-based rationality analysis of agricultural land use implicated that the GFG Project should take cultivation habitat suitability assessment into account.