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We describe a controllable method to fabricate hexagonally close-packedLangmuir–Blodgett (LB) monolayers with stearic acid (SA) asco-surfactant and methanol as co-solvent. The optimal SA concentrationsand volume ratios of chloroform to methanol are 0.8 mg/mL and 3:1for particles of 140 nm, 0.50 mg/mL and 4:1 for particles of 300 nm,and 0.05 mg/mL and 5:1 for particles of 550 nm, respectively. Additionally,SEM detections of the monolayers transferred at different surfacepressures indicate that the monolayers deposited from the binary systemsare more compressible. The experimental results indicate that theinterparticle repulsions and particle–water interactions canbe enhanced without decreasing the particle hydrophobicity by addingSA and methanol; thus, particulate monolayers with large hexagonallyclose-packed domains composed of small silica particles can be successfullyfabricated using LB technique. We propose that the enhanced interparticlerepulsion is attributed to the Columbic repulsion resulting from theattachment of SA molecules to the CTAB modified particles around thethree phase contact line. [ABSTRACT FROM AUTHOR]