The quality of physical education (PE) teaching in colleges and universities is the basis for the development of PE disciplines in colleges and universities, so currently thinking about how to effectively improve the quality of PE teaching in colleges and universities has become the first and foremost problem for many college and university PE departments to solve. In order to solve this problem, it is necessary to build a reasonable and scientific evaluation and monitoring system of PE teaching quality, because only by establishing an effective evaluation and monitoring system of teaching quality can we evaluate and supervise all the PE operation properly and scientifically, and then give feedback in the process of evaluation and supervision, such evaluation and monitoring system can greatly promote the continuous improvement of PE teaching quality in colleges and universities. This is also one of the most effective means to improve the quality of PE and achieve the goal of PE in colleges and universities. The PE teaching quality evaluation in Colleges and Universities is frequently viewed as the multiple attribute group decision making (MAGDM) issue. In this paper, the 2-tuple linguistic neutrosophic number grey relational analysis (2TLNN-GRA) method is built based on the traditional grey relational analysis (GRA) and 2-tuple linguistic neutrosophic sets (2TLNNSs). Then, a numerical example for PE teaching quality evaluation in Colleges and Universities has been given and some comparisons is used to illustrate advantages of 2TLNN-GRA method.