In order to strengthen the evaluation of the quality of sustainable entrepreneurship education in universities, a study was conducted to calculate the correlation degree of the quality of sustainable entrepreneurship education in universities based on the grey correlation algorithm. The study also constructs an evaluation index system and evaluation model from three aspects: the foundation of the entrepreneurship education environment, the allocation of entrepreneurship education resources and the performance of starting an undertaking education result. The result that the evaluation model is more similar to the actual situation indicates that the evaluation indexes have a certain degree of scientificity. The evaluation method of starting an undertaking sustainable education in C&U based on the grey correlation degree algorithm has higher accuracy, recall, and F1 value compared with the traditional way. Therefore, the method has a better evaluation effect for the quality evaluation of entrepreneurship sustainable education in C&U.