Nanocomposites are emerging as a new class of advanced material for many practical applications. Researchers are trying to enhance the properties of polymer-based nanocomposite by tailoring the interface. Studies related to the static and dynamic behavior of nanocomposites are still in an immature state. Due to superior mechanical and thermal properties, hexagonal boron nitride (h-BN) based nanofillers are emerging as exceptional reinforcing agents for high-density polyethylene. Atomistic simulations were used to predict the reinforcing capabilities of defective h-BN nanosheets for polyethylene against shock compressive loading. It was revealed from the atomistic simulations that the geometrical defects in h-BN nanosheets help in improving the interface strength that further leads to enhance the resistance against shock loading of PE nanocomposites. On the other hand, experimental techniques were used to investigate the mechanical behavior of h-BN/PE nanocomposites using the non-functionalized and functionalized interface. The non-bonded interface weakens the interaction and overall load transfer capability and thus restricts the full potential utilization of nanofiller strength. It was captured from the experiments that covalently functionalized interface helps in improving the tensile strength and high strain rate behavior of PE nanocomposites.