Developing modern circular agriculture is one of the important ways to promote agricultural sustainable development, facilitating the achievement of the Sustainable Development Goals adopted by the United Nations. However, when agricultural production operators constructed particular systems, they often lacked accurate data support and parameter matching. Consequently, problems such as unknown input and output, low circulation efficiency, and lack of comprehensive evaluation occurred, increasing challenges for efficient circulation of the systems. Therefore, based on sufficient data collection and field investigation, this research integrated emergy analysis and life cycle assessment to conduct sustainability evaluation on the modern Straw–Sheep–Cropland agro-pastoral circular system. Then the system was optimized by means of coupling parameter adjustment and key technology regulation. The results showed that the whole system required lower total emergy input after optimization. And the total weighted value of potential environmental impacts of the optimized system was 47.12% of that of the original system. Meanwhile, annual environmental service emergy in air, water, and soil was reduced significantly compared with the original one. In general, the optimized system had good performance in reduction, reuse, and controllability, so its sustainability was also high. This research formed a systematic method suitable for evaluating and optimizing the modern agro-pastoral circular system, which provided accurate guidance for the scientific construction and sustainable development of circular agriculture systems.