Considering the importance of the search for sustainability and the growing emphasis given to biofuels, promoted as a promising alternative energy, this study highlights the relevance of research that evaluates sustainability in the bioenergy sector, specifically bioethanol. The present work aims to analyze methodologies aimed at assessing the sustainability of bioethanol using a literature review and, based on this analysis, indicate the most suitable methodology. The most popular methodologies used to assess the sustainability of bioethanol were identified from the bibliographic survey and screened according to pre-established criteria of exclusion, based on keywords, and inclusion, regarding the pillars and biofuel addressed. First, it was found that the studies were conducted in different regional contexts and used different methodologies, which could provide both quantitative and qualitative results. After screening and selection, the evaluation methodologies adopted by each author were analyzed. This analysis made it possible to recognize the factors influencing the choice of methodology, where the suitability of a methodology to the particularities of each case was of great importance. Finally, considering the pre-defined criteria for assessing the sustainability of bioethanol, this paper recommends the GBEP (Global Bioenergy Partnership) methodology as the most appropriate, especially since it was created specifically for the bioenergetic sector and has an accessible application protocol. Lastly, it was also noted that few publications evaluate the sustainability of bioethanol considering its entire three dimensions (social, environmental, and economic), emphasizing the importance of developing more studies with this approach.