In our rapidly urbanizing world, the problem of rurality versus urbanization is becoming a source of concern. Rural tourism development may become a new important stimulus for promoting a sustainable transformation of the farmers’ livelihood. This calls for a smart specialization in rural tourism where the focus is on a balanced rural revitalization strategy. As part of the empirical research, this paper introduces a livelihood sustainability index. This index helps to construct a balanced system for the evaluation of livelihood sustainability achievements in rural tourism destinations. It is based on livelihood capital, livelihood strategy, and the interlinkage between livelihood and environment, in order to dynamically assess the livelihood sustainability of rural households. Taking Huangpi District of the Wuhan area in China as our applied case study, the livelihood sustainability index appears to show over the past years a significant rise, based on a comprehensive index method, an entropy method, and a coupling coordination model. Our findings show that the development of rural tourism has clearly promoted livelihood sustainability. This has inter alia resulted in the accumulation of livelihood capital, an asset of which both social and cultural capital have benefitted greatly; livelihood strategies have also improved, and therefore so have livelihood diversity and stability; and finally, the interlinkage and coordination degree between livelihood and the environment has also changed positively from a primary to intermediate balanced development. However, the livelihood sustainability index in the area concerned is still relatively low, and has not yet reached its possible optimal level. Hence, there is still much room for improvement. Various approaches can be proposed to achieve a more sustainable livelihood, such as enhancing livelihood capital; narrowing the economic gap between farmers by participating in professional tourism activity; establishing the mechanism of industrial integration and the development of rural eco-tourism; and coordinating a balanced development of livelihood and environmental quality.