Low-density polyethylene is the most common polymer for manufacturing containers, bottles, tubes, plastic bags, computer components and so on. There is an urgent need to find solutions for its recycling and reintegration in high volume production components such as non-structural auto applications. The reinforcement of recycled low-density polyethylene with natural fibers represents a solution for the re-use of the recycled low-density polyethylene. However, there is a lack of understanding of how the natural fibers influence the behavior of the bare low-density polyethylene, and furthermore, how the interface between the fibers and the matrix can be controlled in composite to obtain the designed toughness, strength, stiffness and damping. In this sense, the study presents an in-depth analysis of the behavior of three coupling agents used in the chemically functionalized bamboo fibers interface for reinforcing low-density polyethylene composites. Through mechanical tests, the mechanical properties are determined and compared and finally, a correlation between the viscous behavior of the resulted composites and the toughening mechanism is proposed. The conclusion of the study enables a flexible design of polymer composite components fabricated of recycled and non-recycled low-density polyethylene and natural fibers.