In this study, the use of cotton fiber (CF) as a filler in poly(butylene succinate) (PBS) and the effect of silane treatment on the mechanical properties, thermal stability, and biodegradability of PBS/CF composites are investigated. The results showed that the tensile strength of PBS was improved (15%–78%) with the incorporation of CF (10–40 wt%) and was further increased (25%–118%) when CF was treated with a silane coupling agent. Scanning electron microscopy (SEM) observation of the fracture surfaces of PBS/CF composites showed that there was slight improvement in fiber-matrix compatibility. Thermogravimetric (TG) analysis showed that the thermal stability of the composites was lower than that of neat PBS and decreased with increasing filler loading. The biobased carbon content of the composites increased with increasing CF content. The incorporation of CF (with and without silane treatment) in PBS significantly increased the biodegradation rate of the composites.