The correlation of education and unemployment are significant.The main purpose of this study is to analysis the correlation of over-education, under-education and the ratio of unemployment. It used Multi-Regression Analysis to find out the significant factors, and used that model’s significant factors to predict the enrollment of higher education in 89 countries. From the predicted value, it selected the 1/4 top and 1/4 down of 89 countries. That is, in this study are so called over-education group and under-education group in respectively. And our study is to analyze the correlation of the over-education, under-education and unemployment. The results showed that over-education will have higher unemployment, but under-education may be not higher unemployment. The under-education may be lower unemployment. From that finding, some suggestions were given.