Nonlinear electrical properties, such as negative differential resistance (NDR), are essential in numerous electrical circuits, including memristors. Several physical origins have been proposed to lead to the NDR phenomena in semiconductor devices over the last more than half a century. Here, we report NDR behavior formation in randomly oriented graphenelike nanostructures up to 37 K and high on-current density up to 105A/cm2. Our modeling of the current-voltage characteristics, including the self-heating effects, suggests that strong temperature dependence of the low-bias resistance is responsible for the nonlinear electrical behavior. Our findings open opportunities for the practical realization of the on-demand NDR behavior in nanostructures of two- and three-dimensional material-based devices via heat management in the conducting films and the underlying substrates.