With the degeneration of environment and acceleration of urbanization, human environment has attracted great attention worldwide. This paper sets up the Human Settle-ments Environment Index (HEI) model and evaluates the natural environment suitability for Human Settlements in China based on GIS technology. The results show that the HEI of China decreases from southeast to northwest in general, HEI is significantly correlated with population density at grid size and the correlation coefficient (r) between them reaches 0.93, which indicates that natural environment suitability for Human Settlements has a significant influence on population distribution. Most people in China mainly concentrate in areas with high natural environment suitability. The total suitable area is 430.47×104> km2, which ac-counts for nearly 45% of the total land area in China, while the proportion of people living in the area reaches 96.56%. With a population density of 18 people per square kilometer, the critical area is the transitional region for people to live in China. The critical area covers 225.11×104 km2 with a population of 41.12 million. The non-suitable area covers 304.42×104 km2 with a population of only 2.49 million.