UV radiation was used to graft acrylamide (AA) to jute yarn in order to improve the mechanical properties. The physicomechanical properties of the grafted jute yarn were investigated. A series of solutions of different AA concentrations in methanol along with photoinitiator (Irgacure-907, 2%) were prepared. The jute yarns were soaked in the solution for 30 min before radiation. The effect of irradiation time, concentration of monomer on polymer loading, and tensile properties of the jute yarn were studied. The highest polymer loading (22%) and tensile strength (95%) of the yarn were observed when the yarn was treated in 30% AA in methanol with 60 min of UV radiation. The surfaces of both treated and untreated jute were characterized by X-ray photospectrometry, infrared spectroscopy, and environmental scanning electron microscopy, and it was observed that the AA reacted or deposited on the jute surface. A minute amount (1%) of silane monomer [3-(trimethoxysilyl)-propyl methacrylate] was used as an additive in the AA solution to further improve the mechanical properties of jute yarn. Better improvement was achieved by using 1% silane monomer. Water uptake, simulating weathering, and soil degradation tests of untreated and treated yarns were also performed.