Blood-brain barrier (BBB) is a formidable barrier interface that exists between blood and brain, therefore, preventing therapeutic drugs or particles to enter the brain tissue. Nano-medicine is emerging as a prospective way for enhancing pharmaceutical product delivery to the brain with the development of various nano-biotechnologies. In particular, non-viral inorganic layered double hydroxide (LDH) nanoparticles have unique advantages over others in terms of various instinctive properties, such as low cytotoxicity, good biocompatibility and high drug loading capacity. Importantly, previous studies have demonstrated that LDHs can efficiently deliver siRNAs into the neuronal cells, resulting in the knockdown of the target protein. Despite the previous results, two major hurdles still exist before LDHs can be employed as an efficacious central nervous system (CNS) drug delivery system: (i) LDH aggregation upon exposure to the serum environment and (ii) non-specificity in the BBB penetration. This thesis focuses on developing novel engineered LDH delivery system with enhanced suspension stability, redispersion capability and brain targeting ability based on the bovine serum albumin (BSA) coating strategies. Angiopep2 (Ang2) and rabies virus glycoprotein peptide (RVG) are selected as targeting ligands as they can target to the low-density lipoprotein receptor-related protein (LRP) over-expressed on U87 glioma cells and nicotinic acetylcholine receptor (nAchR) on Neura 2a (N2a) cells, respectively. These two ligands can also target the endothelial cells which form the BBB. Moreover, the manganese ions are incorporated into the LDHs system to form magnetic nanoparticles that can act as the potential theranostic agent for simultaneous brain imaging and delivery. First of all, BSA coated LDHs are further crosslinked by glutaraldyhyde (GTA) to improve the suspension stability and residpersion capability based on previous BSA coating strategies. Enhanced colloidal stability and excellent redispersity have been achieved compared with uncrosslinked BSA-LDHs and pristine LDH nanoparticles, with negligible effect on cell cytotoxicity and cell uptake. Thus, the newly developed GTA crosslinking strategy provides a solid LDH-based platform for the following in vitro and in vivo studies. Subsequently, LDHs-based targeting delivery system has been developed by conjugating ligand Ang2 or RVG with LDHs through BSA (Ang2-NPs and RVG-NPs) for brain tumour targeting. In vitro cell uptake shows that the Ang2-NPs and RVG-NPs have enhanced delivery efficiency and demonstrated specificity to relative cells. MTT assay and hemolysis study shows that the newly fabricated various LDH formulations have good blood compatibility and less V