The invention provides a heat radiation material, a heat radiation structure, and preparation methods thereof. The heat radiation material comprises, by weight, 10-30 parts of inorganic heat radiation nano-grade material aqueous slurry, 40-80 parts of aqueous high-molecular resin, 0.5-5 parts of an auxiliary agent, and 5-20 parts of a diluting agent. The inorganic heat radiation nano-grade material aqueous slurry comprises, by weight, 10-25 parts of an inorganic heat radiation nano-grade material, 0.5-20 parts of a bi-functional large-molecular modifier, and 50-100 parts of a solvent. According to the inorganic heat radiation nano-grade material, the bi-functional large-molecular modifier is used in surface modification. Selective absorption and grafting hybridization reaction are carried out on the surface of the inorganic heat radiation nano-grade material, such that coordination self-assembly behaviors of ester bond, silicon-oxygen bond, hydrogen bond, and the like are formed on the surface of the material. Therefore, inorganic heat radiation nano-grade material interface performance is controlled, compatibility and system dispersion stability of the inorganic heat radiation nano-grade material are improved, and better heat radiation performance can be obtained.