With an increasing world population and accelerated urbanization, the development of landscape sustainability remains a challenge for scientists, designers, and multiple stakeholders. Landscape sustainability science (LSS) studies dynamic relationships among landscape pattern, ecosystem services, and human well-being with spatially explicit methods. The design of a sustainable landscape needs both landscape sustainability–related disciplines and digital technologies that have been rapidly developing. GeoDesign is a new design method based on a new generation of information technology, especially spatial information technology, to design land systems. This paper discusses the suitability of GeoDesign for LSS to help design sustainable landscapes. Building on a review of LSS and GeoDesign, we conclude that LSS can utilize GeoDesign as a research method and the designed landscape as a research object to enrich and empower the spatially explicit methodology of LSS. To move forward, we suggest to integrate GeoDesign with LSS from six perspectives: strong/weak sustainability, multiple scales, ecosystem services, sustainability indicators, big data application, and the sense of place. Toward this end, we propose a LSS-based GeoDesign framework that links the six perspectives. We expect that this integration between GeoDesign and LSS will help advance the science and practice of sustainability and bring together many disciplines across natural, social, and design sciences.