Organic-inorganic materials have been widely utilized in various fields as multifunctional materials. Poly(dimethyl siloxane) (PDMS), a typical inorganic polymer, has industrially appealing functions, such as transparency, biocompatibility, and gas permeability; however, it has poor mechanical properties. We incorporated organic-inorganic hybrid elastomers (PDMS-γCD-AAl⊃P(EA-HEMA) (x)) with movable crosslinks, and we utilized hydrogen bonds as reversible crosslinks. The organic polymer poly ethyl acrylate-r-hydroxy ethyl methacrylate (P(EA-HEMA)) penetrated the cavity of triacetylated γ-cyclodextrin (γCD), which was introduced into the side chains of PDMS, and it compounded with PDMS at the nanoscale. Structural studies involving visual and X-ray scattering measurements revealed that movable crosslinks improved the compatibility levels of PDMS and acrylate copolymers. However, macroscopic phase separation occurred when the number of reversible crosslinks increased. Furthermore, studies on the mobility levels of acrylate copolymers and movable crosslinks indicated that the relaxation behaviour of PDMS-γCD-AAl⊃P(EA-HEMA) (x) changed with changing numbers of reversible crosslinks. Introducing reversible crosslinks improved the Young's modulus and toughness values. The movable and reversible crosslinks between the organic and inorganic polymers contributed to the high elongation properties. The design of PDMS-γCD-AAl⊃P(EA-HEMA) (x) incorporated cooperatively movable and reversible crosslinks to achieve high compatibility of immiscible polymers and to control the mechanical properties.