Micro/nano protein fibers have attracted increasing attention owing to their advantageous properties for applications in advanced materials. Traditional preparation methods often suffer from high costs of raw-materials and energy-intensive manufacturing processes, which hinder large-scale production. Herein, we present an innovative low-carbon approach for converting tannery sludge into micro/nano protein fibers. The alkali-oxygen cooking combined with ultrasonic process shown the potential to reduce carbon emissions. The resulting micro/nano protein fibers reinforced the mechanical properties of the cellulose-based films. The maximum tensile force of the cellulose-based film was increased by 55.40%, and the Young’s modulus was increased by 22.92%. The micro/nano protein fibers also imparted remarkable flame-retardant characteristics, as indicated by an increased peak temperature of heat loss and a 21.60% reduction in the peak heat release rate of cellulose-based films. This low-carbon and ecofriendly process utilizing leather tannery sludge not only provides a sustainable source of raw materials but also contributes to the circular economy by repurposing industrial waste.