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Self-healing materials have received increased attention because of their automatic detecting and repairing damage function. In this paper, a novel self-assembly and self-healing bionanocomposite was developed as a coating material for controlled release fertilizers. This nanotechnology-enabled coating is environmentally friendly and highly efficient and possesses a tunable nutrient-releasing characteristic. In the synthesis process, bio-based polyurethane coated urea (BPCU) was prepared by the reaction of bio-polyols with isocyanate. The BPCU was then modified by the layer-by-layer technology to prepare self-assembling modified BPCU (SBPCU). Last, hollow nano-silica (HNS) particles loaded with the sodium alginate (SA) were used to modify SBPCU to fabricate of self-assembling and self-healing BPCU (SSBPCU). The results show that the self-assembled materials were synthesized through electrostatic …