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Low- and middle-income countries have tremendous potential for renewable energy production, including production of renewable carbon from locally prolific crops. In this work, bamboo endemic to West Africa (Bambusa vulgaris) was studied as a feedstock for the production of renewable sugars as the gateway to the local production of biofuels and bio-based chemical products. The effectiveness of delignification and amorphization pretreatments was evaluated, with the observation that quantitative (97 ± 4%) sugar yields could be obtained with a rapid initial hydrolysis rate (82 ± 4 mg g−1 h−1) but only when amorphization was performed following delignification. Experimental measurements and further characterization using 13C solid state nuclear magnetic resonance (NMR) helped establish the importance of amorphization and delignification and explained why the order of these treatments determined their effectiveness. The economics of the bamboo-based process were compared with those projected for corn stover, selected as a well-studied benchmark crop. Because of the higher bamboo growth rate compared with corn stover and the effectiveness of the pretreatment, the projected net present value (NPV) of the bamboo biorefinery was positive ($190 MM, U.S.), whereas the corn biorefinery projected to negative NPV (−$430 MM, U.S.). A socially sustainable framework for deployment of a bamboo biorefinery in a low- or middle-income economy was then proposed, guided by the principle of local ownership and stakeholder buy-in. The findings presented here motivate further investment in development of bamboo cultivation and conversion to sugars as a rapid route to decarbonization of low- and middle-income economies.