Electrostatic assembly is one of the bottom–up approaches used for multiscale composite fabrication. Since its discovery, this method has been actively used in molecular bioscience as well as materials design and fabrication for various applications. Despite the recent advances and controlled assembly reported using electrostatic interaction, the method still possesses vast potentials for various materials design and fabrication. This review article is a timely revisit of the electrostatic assembly method with a brief introduction of the method followed by surveys of recent advances and applications of the composites fabricated. Emphasis is also given to the significant potential of this method for advanced materials and composite fabrication in line with sustainable development goals. Prospective outlook and future developments for micro-/nanocomposite materials fabrication for emerging applications such as energy-related fields and additive manufacturing are also mentioned.

Micro/nanoscale design of composite materials enables alteration of their properties for advanced functional materials. One of the biggest challenges in material design is the controlled decoration of composite materials with the desired functional additives. This study reports on and demonstrates the homogeneous decoration of hexagonal boron nitride (hBN) on poly(methylmethacrylate) (PMMA) and vice versa. The formation of the composite materials was conducted via a low environmental load and a low-energy-consuming, electrostatic nano-assembly method which also enabled the efficient usage of nano-sized additives. The hBN/PMMA and PMMA/hBN composites were fabricated in various size combinations that exhibited percolated and layer-oriented structures, respectively. The thermal conductivity behaviors of hBN/PMMA and PMMA/hBN composites that exhibited good microstructure were compared. The results showed that microstructural design of the composites enabled the modification of their heat-conducting property. This novel work demonstrated the feasibility of fabricating heat-conductive PMMA matrix composites with controlled decoration of hBN sheets, which may provide a platform for further development of heat-conductive polymeric materials.

Despite the availability of nano and submicron-sized additive materials, the controlled incorporation and utilization of these additives remain challenging due to their difficult handling ability and agglomeration-prone properties. The formation of composite granules exhibiting unique microstructure with desired additives distribution and good handling ability has been reported using the electrostatic integrated granulation method. This study demonstrates the feasible controlled incorporation of two-dimensional hexagonal boron nitride (hBN) sheets with alumina (Al₂O₃) particles, forming Al₂O₃–hBN core–shell composite granules. The sintered artifacts obtained using Al₂O₃–hBN core–shell composite granules exhibited an approximately 28% higher thermal conductivity than those obtained using homogeneously hBN-incorporated Al₂O₃ composite granules. The findings from this study would be beneficial for developing microstructurally controlled composite granules with the potential for scalable fabrication via powder-metallurgy inspired methods.