3-(Trimethoxysilyl)propylmethacrylate (silane) solutions of different concentrations in methanol (MeOH) along with the photoinitiator Irgacure 907 were grafted onto jute yarn. Jute yarn grafted with 30% silane under UV radiation for 30 min showed the highest polymer loading (PL) value, 26.2%, with enhanced tensile strength (TS) (259%) and elongation-at-break (Eb) (337%) as compared to untreated yarn. The silanized and virgin jute yarns were characterized by X-ray photoelectron spectroscopy. To attain better performance of jute yarn, the additives (1%) urea, polyvinylpyrrolidone, urethane acrylate, and urethane diacrylate (UDAc) were used in 30% silane. Of the additives used, urea significantly influenced the PL (29%), TS (300%), and Eb (360%) values of the treated jute yarns. Water uptake and the degradation studies were also performed.