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This work reports on the microstructure-controlled formation of interconnected carbon-layered Al 2 O 3 ceramics using carbon nanoparticles (CNP)-alumina (Al 2 O 3 ) composite particles. The Al 2 O 3 micro-particles used in this study were obtained by granulation of nano-sized Al 2 O 3 nanoparticles with an average diameter of 150 nm. Then, CNP-Al 2 O 3 composite was fabricated using an electrostatic assembly method using the granulated Al 2 O 3 and CNP. The decoration of CNP on the surface of granulated Al 2 O 3 was investigated as a function of primary particle size and coverage percentage using a fixed amount of CNP. Notably, an interconnected layer of carbon particles at the interface of Al 2 O 3 that resemble the grain boundaries was obtained. The mechanical properties of the samples obtained with different particle size and CNP coverage on Al 2 O 3 particles were also investigated which presented the possibility to control the mechanical properties through microstructural design of composite ceramic materials.