The study focused on enhancing the feeding value of crop residues through the use of additives for sustainable smallholder feed production. Maize stover was selected due to its abundance and potential to support livestock production in resource-limited communities. The residues were subjected to various treatments including adding urea and molasses aimed at improving their nutritive composition, digestibility, and preservation quality. Results revealed that urea and urea–molasses treatments significantly increased crude protein levels while reducing fiber content, thereby improving the overall nutritional profile. The combined urea–molasses treatment yielded the best balance between nutrient enhancement, palatability, and long-term storage stability. The findings underscore the potential of additive treatments as cost-effective strategies for transforming low-value crop residues into nutritionally improved feed resources. This approach promotes sustainable livestock feed production and supports food security efforts under Zimbabwean smallholder farming systems. It also supports the country’s Vision 2030, from where the country is poised to be a middle income economy by then.