Inner Mongolia Autonomous Region (IMAR) is one of China’s strategic energy bases for the 21st century. While bioenergy in IMAR may play an important role in securing future energy supply, little research has been done so far, particularly for crop stalk resources as a potential source of bioenergy in this region. In this study we systematically analyzed the temporal and spatial patterns of crop stalk resources, evaluated the bioenergy potential of crop stalk resources, and explored possible pathways of developing stalk-based energy strategies in Inner Mongolia. Our results show that the total crop stalk yield in IMAR increased consistently from 1980 to 2008, with an average annual increase of 16.3%. Between 2004 and 2008, 26.14 million tons of crop stalks were produced each year in IMAR, 8.82 million tons of which could be used for biofuel production. Grain crops contributed most to the total amount of stalks for energy production, of which corn stalks were the largest contributor, accounting for 62% of the total crop stalk yield. Based on the current trend, crop stalk yields may continue to increase in the future. Geographically, the abundance of biofuelable crop stalk resources, either on a per capita or per unit of area basis, had a spatial pattern of “high on East and West and low in the middle”. Our findings suggest that IMAR has the potential for developing stalk-based bioenergy to improve its current overwhelmingly coal-dominated energy structure. However, more detailed and comprehensive studies are needed to figure out how exactly such bioenergy development should be carried out in a way that would promote the regional sustainability of Inner Mongolia – i.e., simultaneously providing social, economic, and ecological benefits.