This research was aimed to investigate the impact of the COVID-19 pandemic on the green entrepreneurial intention of college students through green entrepreneurial self-efficacy, optimism, ecological values, and social responsibility, as well as the mediating role of green entrepreneurial motivation. This study used structural equation model to test the hypothesis on samples of 410 Chinese colleges’ students. COVID-19 has a strong beneficial effect on green entrepreneurial self-efficacy, optimism, ecological values, and social responsibility, according to the research findings. Optimism and social responsibility also were found to have a significant positive impact on green entrepreneurial self-efficacy. Moreover, green entrepreneurial motivations moderated the relationship between optimism, ecological values, social responsibility, and green entrepreneurial intention in a positive and significant way. Finally, the findings indicate that a significant positive correlation exists between green entrepreneurial self-efficacy and optimism, as well as a significant positive correlation between ecological values and social responsibility.