Abstract: In the digital economy, corporate entrepreneurship has become an important way for large enterprises to explore new opportunities and build new advantages, which has strategic significance for high-quality development in the new development era. However, most large enterprises in China do not carry out corporate entrepreneurship smoothly and have low entrepreneurial activity. Therefore, how to stimulate corporate entrepreneurship of large enterprises in the digital economy to achieve high-quality development has become an important issue. Based on the perspective of organization-environment interaction, this study constructs a theoretical framework of corporate entrepreneurship in the digital economy, and conducts a configuration analysis of 49 large Chinese enterprises using the fuzzy-set qualitative comparative analysis method. The results show that: (1) there are three matching modes for high-level corporate entrepreneurship in the digital economy, including “resource-capability autonomy”, “resource-government complementarity”, and “organization-environment synergy”; (2) Under certain combinations, organizational and environmental conditions can promote high levels of corporate entrepreneurship through complementary combination or equivalent substitution. As a key condition, digital resource endowment plays a more universal role in the process; (3) State-owned enterprises and private enterprises have exclusive paths to high-level corporate entrepreneurship. State-owned enterprises tend to prefer the “government driven-capability supported” model, while private enterprises focus on developing the “capability led-internal oriented” model. The theoretical contributions highlight as follows: (1) we construct a theoretical framework of corporate entrepreneurship in the digital economy, reveal the synergistic driving mechanism of organizational and environmental conditions integrating digital elements on corporate entrepreneurship in large enterprises, and promote the research on the antecedents of corporate entrepreneurship in the digital context; (2) we identify the complementary matching effect between digital resources and digital capabilities, reveal the path mechanism of their orchestration linkage leading to high-level corporate entrepreneurship, and expand the application of resource orchestration theory in corporate entrepreneurship research; (3) we refine the exclusive configurations of high-level corporate entrepreneurship in state-owned enterprises and private enterprises, reveal the heterogeneity and complexity of the driving mechanism of corporate entrepreneurship, and deepen the applicable boundaries of different paths of corporate entrepreneurship.