Yes / In this paper, two types of nano carbon materials including 0D nano carbon black and 2D graphene are assembled through electrostatic adsorption to develop smart cement-based composites. Owing to their excellent mechanical, electrical properties and synergistic effect, self-assembled 0D/2D nano carbon materials can form toughening and conductive networks in cement-based materials at low content level and without changing the preparation process of conventional cement-based materials, thus endowing cement-based materials with smart and multifunctional properties including high toughness, self-sensing property to stress/strain and damage, shielding/absorbing property to electromagnetic wave. The developed smart cement-based composites with self-assembled 0D/2D nano carbon materials have promising application in the fields of oil well cementing, structural health monitoring, and electromagnetic protection and anti-electromagnetic pollution. It can therefore conclude that electrostatic self-assembled 0D/2D nano carbon materials provide a simple preparation method and excellent composite effect for developing nano cement-based materials, which can be applied in large-scale infrastructures. / The National Science Foundation of China (51908103) and the China Postdoctoral Science Foundation (2019M651116).