Access to energy services is a priority for sustainable economic development, especially in rural areas, where small- and medium-sized enterprises have many difficulties in accessing reliable and affordable electricity. Western African countries are highly dependent on biomass resources; therefore, understanding the potential of bioenergy from crop residues is crucial to designing effective land-management practices. The assessment of the capability to use crop residues for electricity production is particularly important in those regions where agriculture is the dominant productive sector and where electrification through grid extension might be challenging. The objective of this work was to guide the development of sustainable strategies for rural areas that support energy development by simultaneously favouring food self-sufficiency capacity and environmental benefits. These complex interlinkages have been jointly assessed in the Senegal river basin by an integrated optimization system using a cropland–energy–water-environment nexus approach. The use of the nexus approach, which integrates various environmental factors, is instrumental to identify optimal land-energy strategies and provide decision makers with greater knowledge of the potential multiple benefits while minimizing trade-offs of the new solutions such as those connected to farmers’ needs, local energy demand, and food and land aspects. By a context-specific analysis, we estimated that, in 2016, 7 million tons of crop residues were generated, resulting in an electricity potential of 4.4 million MWh/year. Several sustainable land-energy management strategies were explored and compared with the current management strategy. Our results indicate that bioenergy production from crop residues can increase with significant variability from 5% to +50% depending on the strategy constraints considered. An example analysis of alternative irrigation in the Guinea region clearly illustrates the existing conflict between water, energy, and food: strategies optimizing bioenergy achieved increases both for energy and food production (+6%) but at the expense of increasing water demand by a factor of nine. The same water demand increase can be used to boost food production (+10%) if a modest decrease in bioenergy production is accepted (−13%).