This study aims to explore the roles of Chinese ICT enterprises in promoting the ICT industry ecosystem in education in China, and construct a structural model of a healthy ICT industry ecosystem in education. After examining ICT demands in education, this study adopts a multiple case studies methodology. Fifty-five employees from five enterprises (iFLYTEK, Tencent, EIST, Sh-tz and Beijing Tstudy) participated in this research. This study mainly adopted qualitative research methods to collect data, including interviews and documentations (secondary data). Quantitative data from a questionnaire were also collected to complement the qualitative data. To ensure reliability and validity, data from multiple sources were triangulated to address the same research question. The result in-depth illustrates the products and roles of three cases which are iFLYTEK, Tencent and EIST, and further reveals the roles of ICT enterprises. Based on the results, this study divides ICT enterprises into Small and Medium-sized enterprises with less roles, and Large-Scale Enterprises with more roles, and puts forward a structural model of a healthy ICT industry ecosystem in education. This study provides feasible recommendations for governments, consumers and micro and macro directions and paths for the strategic choices of enterprises. This work offers guidance to relevant researches and practices.