The aim of this study was to explore and construct spatial indicators suitable for green café ambience. The indicators were further empirically verified. A three-round questionnaire survey, based on the Delphi method, was conducted with 15 experts, including university professors (food and beverage services management and interior environmental design), café operators, and personnel from government agencies. Data were collected, and the results on the characteristics of the repeated feedback from the experts were convergent. Thirty-six indicators suitable for the design of green café ambience were extracted, of which 17 were verified by actual cafés as highly operable. The five-sense indicators of sustainable green ambience design obtained in this study can facilitate positive customer experiences and enhance the appeal of maintaining sustainable green trends for cafés. These indicators can also provide references for café operators in business planning and green café ambience design.