The invention belongs to the field of organic-inorganic composite materials and relates to layered double hydroxides (LDHs) loading highly-dispersed fullerenes and a preparing method of the LDHs. The method of the LDHs includes the steps of firstly preparing precursors of the LDHs, then preparing naphthylacetic acid intercalated LDHs, forming a hydrophobic environment containing a plurality of naphthalene groups in layers of naphthylacetic acid intercalated LDHs, and finally fixing the fullerenes into the layers of the LDHs. According to the LDHs loading the highly-dispersed fullerenes and the preparing method of the LDHs, the fullerene and naphthylacetic acid intercalated LDHs are of supramolecular structures, crystal structures of the LDHs are the crystal structures of layered double hydroxide-like materials, and the chemical formula is [ (M2+)1-x(M3+)x(OH)2 ]x+(NAA-)x(C60)y-water(1 / m), wherein x=0.25-0.33,y=0.05-0.1, m=3-6, the m relates to the number of crystal water molecules in the layers, M2+ relates to a divalent metal ion, and M3+relates to a trivalent metal ion of Al3+. According to the LDHs loading the highly-dispersed fullerenes and the preparing method of the LDHs, due to high interaction forces between the fullerenes (C60) and the naphthylacetic acid, the prepared fullerene and naphthylacetic acid intercalated LDHs have stable intercalation structures and can be used for preparing non-linear optics materials, strong magnetic materials and the like, and the preparing method is simple, practicable and easy to operate.