The essence of cross-border search behavior of university teachers is to break through their own organization and knowledge boundary to search and innovate knowledge. According to the analysis of 208 college teachers, this paper constructs a mechanism model of the influence of organizational innovation atmosphere on Teachers’cross-border search behavior. The results show that: ① organizational innovation atmosphere and self-efficacy have a positive impact on Teachers’cross-border search behavior; ② self-efficacy partially mediates the relationship between organizational innovation atmosphere and cross-border search behavior; ③ cross-border communication and training play a moderating role in the relationship between self-efficacy and cross-border search behavior. Based on the above findings, this paper puts forward suggestions to promote the cross-border search behavior of university teachers from three aspects: focusing on the cultivation of outstanding talents in the new era, building a full career gold teacher training system, as well as building an intelligent data fusion platform, which provides enlightenment and reference for promoting the cross-border development of teachers in the new era and improving the quality of new engineering talent training.