Pillar-like structures of nanodiamonds on silicon substrate are self-assembled for the first time by pulsed spray technique. This technique allows to deposit nanodiamond layers by using high quality nanocrystals of 250 nm dispersed in 1,2-dichloroethane solvent. The analysis of 2D/3D confocal and atomic force microscopy images evidences the presence of the self-assembled pillar-like structures distributed in an irregular way. The proposed method is simple, easy and cheap, and does not require complex growth processes or structured materials, ideal for upscaling towards industrial biochip implementation and photonic applications. The suggested formation mechanisms of self-assembly are based on the so-called coffee stain effect, i.e. on the time evolution of DCE evaporation.