We determine the frictional figures of merit for a pair of layered honeycomb nanostructures, such as graphane, fluorographene, MoS 2 and WO 2 moving over each other, by carrying out ab initio calculations of interlayer interaction under constant loading force. Using the Prandtl-Tomlinson model we derive the critical stiffness required to avoid stick-slip behavior. We show that these layered structures have low critical stiffness even under high loading forces due to their charged surfaces repelling each other. The intrinsic stiffness of these materials exceeds critical stiffness and thereby the materials avoid the stick-slip regime and attain nearly dissipationless continuous sliding. Remarkably, tungsten dioxide displays a much better performance relative to others and heralds a potential superlubricant. The absence of mechanical instabilities leading to conservative lateral forces is also confirmed directly by the simulations of sliding layers. © 2012 American Physical Society.