A high-efficiency biosorbent based on the low-priced jute fiber was developed, characterized, and applied to remove the emerging organic contaminant diclofenac from aqueous solutions. Jute fiber was treated by NaOH (named AJF) followed by graftingdifferent amounts of trimethyl[3-(trimethoxysilyl) propyl] ammonium chloride (named AJF-TTSAC). The composition, morphology, porosity, and adsorption features of the neat and modified jute fiber were evaluated and compared. The surface of neat JF was smooth, nonporous, and free of cracks. NaOH treatment increased the fibrillation, created cracks and grooves, and increased the oxygen content, total pore volume, and surface area. In comparison to AJF, grafting TTSAC filled in the crevices, grooves, and spaces between fibrillates, and decreased the total pore volume and surface area. The adsorption of diclofenac by the neat and modified JF occurred at highly acidic pHo and peaked at pHo 3. Among the neat and modified JF, AJF-TTSAC5 was the most efficient followed by AJF. The efficiency of AJF and AJF-TTSAC5 was highest using 1.00 g/L, at 35 °C and was not affected by the presence of NaCl. The Elovich, pseudo-first-order, and pseudo-second-order models described the adsorption kinetic satisfactorily with the marginal advantage of Elovich for AJF and pseudo-second-order for AJF-TTSAC5. The isotherm study exposed the multilayer and physisorption nature of the adsorption of diclofenac onto AJF and AJF-TTSAC5. The Langmuir monolayer saturation capacity of AJF-TTSAC5 was 37.43 mg/g which revealed its great potential relative to other adsorbents in the literature. The AJF and AJF-TTSAC5 were easily regenerated using distilled water and kept good performance for 5 repetitive cycles.