Carborane-intercalated layered double hydroxide nanohybrids (CB-LDH) and a magnesium ferrite (MF) supported-CB-LDH core-shell nanocomposite (CB-LDH@ MF) are reported. The preparation of nanohybrids were carried out by exchanging the interlayer nitrate groups of Mg-Al-NO3-LDH with monothiolo- carborane (SCB), 1-methyl-2-carboxyl-o-carborane (MeCB), 1-phenyl-2-carboxyl-o-carborane (PhCB) and 1,12-dicarboxyl-p-carborane (COOHCB) molecules. A magnetic core-shell nanocomposite was further prepared by supporting the COOHCB-LDH nanohybrid on MF nanoparticles. The obtained materials were characterized by means of several physical and chemical methods. Chemical compositions were determined by elemental analysis, ICP measurements and SEM-EDX data. Structural characterization was performed with powder-XRD, FTIR and magnetization measurements. Morphological analyses were conducted with electron microscopy imaging (SEM and TEM). Thermal stabilities were investigated by TGA/ DTA. Carborane release from LDH layers was tested by tracing the amount of boron species transferred to the solution phase with ICP-MS measurements. The results verified that the prepared nanohybrids have the potential to be used in Boron Neutron Capture Therapy (BNCT) and magnetically targeted-BNCT applications.