Contemporary R D activities aimed at enhancing the delivery of insoluble food bioactives have focused on the development of sustainable nanomaterials. In this study, a novel self-assembled complex of cationic biopolymer chitosan (CS) and anionic biosurfactant surfactin (SF) was successfully developed via the nanoprecipitation method for the encapsulation of bioactive curcumin (Cur). Complex formation is driven by a synergistic interplay of electrostatic and hydrophobic interactions as revealed by comprehensive physicochemical and thermodynamic investigation. An amorphous form of Cur was loaded in the CS-SF nanocomplex, as evidenced from X-ray diffraction pattern and differential scanning calorimetry. The CS-SF-Cur nanocomplex exhibited spherical core-shell morphology as revealed by FESEM and TEM imaging with a hydrodynamic diameter of 302.37 ± 51.98 nm and a polydispersity index of 0.34 ± 0.1. The encapsulation and loading efficiencies of Cur were 86.1 ± 0.21