Nanodiamonds were immobilized into chitosan biopolymer to fabricate hybrid microcapsules via electrospraying technique. Previously optimized electrospraying parameters for the formulation of chitosan microcapsules were adjusted to accommodate the immobilized nanodiamonds and maintain a suitable capsule size for the novel hybrid. The yield and entrapment efficiency of the composite microcapsules, including capsule strength were analyzed. The chemical structure, elemental composition, crystalline phases, size distribution, surface morphology, and thermal stability of microcapsules were assessed by Fourier transform infrared (FTIR) spectroscopy, energy dispersive x-ray spectroscopy (EDX), X-ray diffraction (XRD), scanning electron microscopy (SEM) and thermogravimetric analysis (TGA), respectively. The results demonstrated a 39 % reduction in the size of composite microcapsules and sphericity improvement after the adjustment. There was a general observation of good yield and immobilization efficiency with the maximum at 96.2 % and 93.8 % for yield and entrapment efficiency, respectively. Characterized composite microcapsules showed desirable morphology, good thermal stability and enhanced mechanical strength, and overall successful fabrication of the hybrid microcapsules. The hybrid microcapsules were subsequently loaded in epoxy resin and coated on a steel substrate to assess their self-healing and anticorrosion abilities. Cross-scratched coating samples were monitored visually for healing efficiency and further analyzed with EIS and potentiodynamic polarization. The self-healing coating showed efficient self-healing and anticorrosion capabilities with a healing efficiency of 97.3 % and a protection efficiency of 99.4 %, confirming the unique feature of the hybrid chitosan-nanodiamonds microparticles for self-healing and anticorrosion purposes.