Solar photovoltaic (PV) generation will play a crucial role in the global clean energy transition toward carbon neutrality. While the development of solar PV generation has been explored in depth, the development of high-proportion solar PV generation has yet to be discussed. Considering the back force of the constraint of achieving carbon neutrality within the specified timeframe, this paper establishes a unified, multi-dimensional, and achievable framework through which to perform a system analysis for exploring the potential risks and challenges involved in the development process of high-proportion solar PV generation and investigating possible pathways to fostering the development of high-proportion solar PV generation. The results show that the critical risks and challenges include a low conversion efficiency, poorer resource endowment, more limited land resources, a low use of rooftop resources, an increasing complexity of power system scheduling, and low public awareness. These challenges have emerged with the development of solar PV generation in China and the aim of developing high-proportion solar PV generation. Based on our findings, possible pathways toward developing high-proportion solar PV generation have been determined, including promoting the research and development of higher PV efficiency, determining the optimal development sequence of solar resources, tapping the potential of land resources, increasing the use of rooftop resources, improving the resilience of the power system, and enhancing the public awareness of deploying solar PV generation. Finally, recommendations are proposed to optimize policy formulation for stimulating the high-quality development of high-proportion solar PV generation for carbon neutrality in countries including China.