Intensive agriculture in China over recent decades has successfully realized food security but at the expense of negative environmental impacts. Achieving green transformation of agriculture in China requires fundamental restructuring of cropping systems. This paper presents a theoretical framework of theory, approaches and implementation of crop diversification schemes in China. Initially, crop diversification schemes require identifying multiple objectives by simultaneously considering natural resources, limiting factors/constraints, and social and economic demands of different stakeholders. Then, it is necessary to optimize existing and/or design novel cropping systems based upon farming practices and ecological principles, and to strengthen targeted ecosystem services to achieve the identified objectives. Next, the resulting diversified cropping systems need to be evaluated and examined by employing experimental and modeling approaches. Finally, a strategic plan, as presented in this paper, is needed for implementing an optimized crop diversification in China based upon regional characteristics with the concurrent objectives of safe, nutritious food production and environmental protection. The North China Plain is used as an example to illustrate the strategic plan to optimize and design diversified cropping systems. The implementation of crop diversification in China will set an example for other countries undergoing agricultural transition, and contribute to global sustainable development.