In recent years, crossover services have attracted wide attention as an emerging service mode in the modern service industry. Crossover services can offer values that cannot be provided by single-domain services, and they usually need to cross the boundaries of domains, organizations, and processes, which puts forward more challenges for requirements modeling and analysis under the crossover scenarios. Given the characteristics of crossover services, the authors propose a value-driven meta-model framework from multiple viewpoints to support the requirements analysis of crossover services, which consists of three parts: a value network, a goal network, and a service network. Based on the proposed meta-model framework, a value-driven crossover service modeling tool is developed to help requirements analysts in requirements analysis and design, and a case study is presented to illustrate the usage of the proposed approach. Finally, we evaluate our methods and tools using a controlled experiment, and the experimental results show the effectiveness of the approach.