The research on the sustainability evaluation of innovation and entrepreneurship education for clean energy majors in colleges and universities can not only cultivate more and better innovative and entrepreneurial talents for the development of sustainable energy but also provide a reference for the sustainable development of innovation and entrepreneurship education for other majors. To achieve systematic and comprehensive scientific evaluation, this paper proposes an evaluation model based on SPA-VFS and Chaos bat algorithm to optimize GRNN. Firstly, the sustainability evaluation index system of innovation and entrepreneurship education for clean energy major in colleges and universities is constructed from the four aspects of the environment, investment, process, and results, and the meaning of each evaluation index is explained; Then, combined with variable fuzzy set evaluation theory (VFS) and set pair analysis theory (SPA), the classical evaluation model based on SPA-VFS is constructed, and the entropy weight method and rank method are coupled to obtain the index weight. The basic bat algorithm is improved by using Tent chaotic mapping, and the chaotic bat algorithm (CBA) is proposed. The generalized regression neural network (GRNN) model is optimized by CBA, and the intelligent evaluation model based on CBA-GRNN is obtained to realize fast real-time calculation; finally, a numerical example is used to verify the scientificity and accuracy of the model proposed in this paper. This study is conducive to a comprehensive evaluation of the sustainability of innovation and entrepreneurship education for clean energy major in colleges and universities, and is conducive to the healthy and sustainable development of innovation and entrepreneurship education for clean energy major in colleges and universities, so as to provide more innovative and entrepreneurial talents for the clean energy industry.