The analysis of the relationship between regional resources and environment and human activities plays an important role in sustainable regional development. This study proposes the pressure–capacity–governance (PCG) model, an analytic framework for the assessment of the resources and environmental pressure (REP), carrying capacity (RECC) and governance (REG) levels over a large watershed scale, with the Yangtze River Economic Belt (YREB) as the study area. A limiting factor analysis is used to recognize the limiting factors of the regional RECC. The coupling analysis of resources and environmental pressure–capacity–governance identifies the regional potential and utilization direction. The research results are as follows. (1) The REP, RECC and REG levels of the YREB exhibit spatial differences. The REPs of the upper reaches are lower than those of the lower reaches, which does not match the RECC but matches the REG levels. (2) The proportions of unused land, water resources, and atmospheric environmental quality are the main limiting factors of the regional RECC. (3) The PCG analysis framework is used as the basis to divide the YREB into several subareas to analyse the resources and environmental potential carrying capacity and utilization direction of different types of region. This research may provide decision-making references for regional sustainable development at the large watershed scale.