In this investigation, we studied the impact toughness and viscoelastic behavior of polypropylene (PP)-jute composites. In this study, we used viscose fiber as an impact modifier and maleated PP as a compatibilizer. The toughness of the composites was studied with conventional Charpy and instrumental falling-weight impact tests. The composites' viscoelastic properties were studied with dynamic mechanical analysis. The results show that the incorporation of viscose fibers improved the impact strength and toughness to 134 and 65% compared to those of the PP-jute composites. The tan δ peak amplitude also increased with the addition of the impact modifier and indicated a greater degree of molecular mobility. The thermal stability of the composites was evaluated with thermogravimetric analysis. The addition of 2 wt % maleated polypropylene (MAPP) to the impact-modified composite improved the impact strength and toughness to 144 and 93%, respectively. The fiber-matrix morphology of the fracture surface and the Fourier transform infrared spectra were also studied to ascertain the existence of the type of interfacial bonds. Microstructural analysis showed the retention of viscose fibers in the composites compared to the more separated jute fibers.