In this work, mechanochemical pretreatment of Bambusa vulgaris is evaluated for waste-free production of renewable sugars for subsequent fermentation. After a 60 min mechanochemical pretreatment followed by enzyme hydrolysis at 50 °C, 62% of the available carbohydrate can be recovered as fermentable sugars, primarily in the form of glucose and xylose. Structural and chemical analysis finds that mechanochemical pretreatment increases accessible surface area and amorphizes the crystalline cellulose present in bamboo, both of which increase reactivity. The experimental results are then used for a systems-level analysis of ethanol production in Nigeria. The energy required for mechanochemical pretreatment is estimated to be 0.5–5.6 MJ per kg of bamboo; this energy can be provided by solar power, while still satisfying existing needs for stationary power. Ethanol production on marginal land alone is projected to be sufficient to replace nearly 80% of Nigeria's current gasoline usage while reserving sufficient land area for solar power generation to meet current electricity needs, meaning that bamboo cultivation followed by mechanochemical pretreatment can play an important role for utilizing locally available resources without generation of new chemical wastes.