The invention discloses organic-inorganic hybrid particles, a preparation method of the organic-inorganic hybrid particles and application of the organic-inorganic hybrid particles to modification of cement-based materials. The particles comprise organic components and inorganic components, and the inorganic components and the organic components are mutually connected in a crossed manner through covalent bonds instead of core-shell structures. The organic-inorganic hybrid particles have the advantages that the organic components are used for improvement of mechanical properties of the cement-based materials; by complete connection of the organic components with CSH (calcium silicate hydrate) particles through the inorganic components and the covalent bonds, toughness efficacy of the organic components is promoted; in addition, the more the organic-inorganic hybrid particles are doped into the cement-based materials, the more evidently the mechanical properties of the cement-based materials are improved.