The electronic structures and magnetic properties of graphene nanoflakes (GNFs) exposed to an organo-silane precursor [tetra-methyl-silane, Si(CH 3) 4 ] were studied using atomic force microscopy, electron field emission (EFE), x-ray photoelectron spectroscopy (XPS), and magnetization. The result of XPS indicates that silyl radical based strong covalent bonds were formed in GNFs, which induced local structural relaxations and enhanced sp 3 hybridization. The EFE measurements show an increase in the turn-on electric field from 9.8 V/lm for pure GNFs to 26.3 V/lm for GNFs:Si having highest Si/(Si þ C) ratio (ffi 0.35) that also suggests an enhancement of the non-metallic sp 3 bonding in the GNFs matrix. Magnetic studies show that the saturation magnetization (Ms) is decreased from 172.53 Â 10 À6 emu/g for pure GNFs to 13.00 Â 10 À6 emu/g for GNFs:Si with the highest Si/(Si þ C) ratio 0.35, but on the other side, the coercivity (Hc) increases from 66 to 149 Oe due to conversion of sp 2 ! sp 3-hybridization along with the formation of SiC and Si-O bonding in GNFs. The decrease in saturation magnetization and increase in coercivity (Hc) in GNFs on Si-functionalization are another routes to tailor the magnetic properties of graphene materials for magnetic device applications.