This paper introduces a methodological framework for assessing the sustainability of solid biofuels in Mexico. The designed framework comprises 13 normalized indicators and two diagnostic studies, covering the economic, social, environmental, and institutional sustainability dimensions, and their intersections. Indicators are normalized using the concept of load capacity of a system, similarly to the planetary boundaries. Thus, the graphical representation of results facilitates their multidimensional analysis. The framework was applied to three case studies: traditional fuelwood in rural households, charcoal for restaurant grilling, and electricity cogeneration from sugarcane bagasse. This was part of an iterative process of testing and refining the framework and simultaneously demonstrating its application in the Mexican bioenergy context. This led to the conclusion that the resulting framework (a) provides a useful, quantitative, and comprehensive overview of both broad and specific sustainability aspects of the assessed system; (b) requires a balance of accessible but also scattered or sensitive data, similarly to most existing frameworks; (c) is highly flexible and applicable to both modern and traditional solid biofuels; and (d) is simple to communicate and interpret for a wide audience. Key directions for improvement of the framework are also discussed.The online version contains supplementary material available at 10.1007/s12155-021-10365-2.