Access to electricity is a crucial factor in boosting the economic, environmental, and social development of developing nations. This study presents a framework that combines and integrates indicators and methods to determine the most sustainable solution for off-grid electrification, focusing on the Mavumira village in Mozambique. The framework covers various methods including input–output, life cycle assessment based on SimaPro, and HOMER. Data for the analysis were obtained from the literature, the HOMER database, and the ecoinvent database. Our results show that renewables are the most sustainable solutions compared to diesel-only options as they can lower the cost of electricity by 20%, create approximately 26 more local jobs, reduce about 77% of greenhouse gas emissions caused by burning fossil fuels, and have higher values of HDI than diesel-only options. Using the MCDA (TOPSIS method), we found that the future renewable scenario ranked highest with a closeness value of one, while the diesel-only option ranked third and fourth on a ranking scale from 1 to 4. This study concludes with future research directions for applying the framework to other case studies using different renewable technologies like wind, hydropower, and biomass in villages with similar characteristics to Mavumira. The novelty of this study lies in applying various methods and indicators to analyze the sustainability of an implemented project for the current and future scenarios. Additionally, the framework presented in this study would assist policymakers in selecting the best energy alternatives for rural electrification.