The invention discloses a nano high-resilience composite material for children's toys and a preparation method thereof. The composite material is prepared from the following raw materials in parts byweight: 75-85 parts of polyether polyol, 30-45 parts of MDI, 1.2-1.8 parts of stannous octoate, 5-7 parts of dipropylene glycol, 25-38 parts of thermoplastic elastomer, 20-40 parts of polylactic acid,3-5 parts of cross-linking agent, 10-25 parts of bamboo charcoal fiber, 5-8 parts of pentaerythritol, 1-3 parts of gum base, 2-5 parts of polymethylene polyphenyl isocyanate, 0.5-1.5 parts of phosphoric acid, 2-5 parts of glycerol, 8-15 parts of nano filler and 0.5-1.5 parts of water. The nano high-resilience composite material prepared by adopting the reasonable formula and the preparation method has relatively high tensile strength, good mechanical property, high resilience rate and excellent resilience performance, and is suitable for manufacturing toys for children.