Globally, over 4.5 million reconstructive surgeries are conducted each year to address a range of causes, including accidents, cancer procedures, and cosmetic enhancements. Global Burden Disease data analysis revealed that approximately 1.71 billion people worldwide have musculoskeletal conditions. Consequently, there is a need for effective biomaterial for bone treatment and replacement. The unique characteristics of bone, its constituent phases, and structural relationships at various hierarchical levels are complex. Therefore, replicating it artificially to achieve biomaterials with properties comparable to bone has proven challenging. For this reason, allograft remains a gold standard for treating bone-related disorders. There is a need to develop synthetic materials similar to natural bone. Bone is a nanocomposite material made up of inorganic and organic counterparts. The organic component primarily comprises calcium phosphate (CaP), while the organic content predominantly comprises collagen. The inorganic content of bone is synthesized through a mitochondrial-dependent cellular mechanism in the form of amorphous calcium phosphate (ACP), which is further nucleated to lowcrystalline apatite (Ap) in the presence of collagen. In mitochondria, the ACP is associated with an organic compound that regulates interfibrillar collagen mineralization. The side chains of an organic compound (carboxylate or hydroxyl groups) allow interaction with CaP by surface adsorption. The organic compound delay CaP crystallization can be due to retarding the transformation rate (crystallization) of ACP to Ap or interaction with the crystalline phase by inhibiting the growth of nuclei. Therefore the organic compound becomes a key player in regulating interfibrillar collagen mineralization. The Doctoral Thesis aims to develop small organic molecule-containing ACPs and their nanocomposites as bone substitute materials for improved bone regeneration. Based on this, five synthetic SOMs have been selected with diverse functional groups and used for the development of SOM-containing ACPs. These SOMs are also naturally present in mitochondria and play a role in bone regeneration. The primary goal was to develop a wet chemical synthesis route for the synthesis of SOMcontaining ACP and analyze the impact of SOM on ACP's physiochemical properties (particle size, morphology, true density, specific surface area, and transformation kinetics) and cytocompatibility. Synthetic SOM-containing ACPs were used as inorganic fillers in an organic matrix to develop nanocomposite scaffolds. Nanocomposite bioink was developed by adding the SOM-containing ACPs as an inorganic filler in an alginate-dialdehyde-gelatin (ADA-GEL) organic matrix wherein citrate-containing ACP (ACP_CIT) was effective in maintaining the structural integrity of the bioprinted scaffolds. Subsequently, a single-network (SN) nanocomposite hydrogel consisting of gelatin methacrylate (GELMA) and ACP_CIT was developed using chemical crosslinking. Afterwards, a double network (DN) nanocomposite hydrogel of polyacrylamide (PAM), Pluronic P123, GELMA, and ACP_CIT was formulated. Initially, the effect of P123 on the mechanical properties of PAM-GELMA hydrogel was evaluated, followed by analyzing the effect of ACP on the mechanical and rheological properties of PAM-GELMA-P123 hydrogels. Subsequently, their shape memory effect was also evaluated. In conclusion, all the synthesized ACPs and their nanocomposite bioink, SN, and DN hydrogels demonstrate cytocompatibility, suggesting their potential use in bone tissue regeneration applications.