This study aimed to develop injectable chitosan oligosaccharide (COS) and bovine hydroxyapatite (BHA) hybrid biocomposites, and characterise their physiochemical properties for use as a dental pulp-capping material. The COS powder was prepared from chitosan through hydrolytic reactions and then dissolved in 0.2% acetic acid to create a solution. BHA was obtained from waste bovine bone and milled to form a powder. The BHA powder was incorporated with the COS solution at different proportions to create the COS–BHA hybrid biocomposite. Zirconium oxide (ZrO2) powder was included in the blend as a radiopacifier. The composite was characterised to evaluate its physiochemical properties, radiopacity, setting time, solubility, and pH. Fourier-transform infrared spectroscopic analysis of the COS–BHA biocomposite shows the characteristic peaks of COS and hydroxyapatite. Compositional analysis via ICP-MS and SEM-EDX shows the predominant elements present to be the constituents of COS, BHA, and ZrO2. The hybrid biocomposite demonstrated an average setting time of 1 h and 10 min and a pH value of 10. The biocomposite demonstrated solubility when placed in a physiological solution. Radiographically, the set hybrid biocomposite appears to be more radiopaque than the commercial mineral trioxide aggregate (MTA). The developed COS-BHA hybrid biocomposite demonstrated good potential as a pulp-capping agent exhibiting high pH, with a greater radiopacity and reduced setting time compared to MTA. Solubility of the biocomposite may be addressed in future studies with the incorporation of a cross-linking agent. However, further in vitro and in vivo studies are necessary to evaluate its clinical feasibility.