Organic-inorganic hybrid zeolite materials containing an organic framework have been synthesized by partially superseding a lattice oxygen atom by a methylene group. The use of methylene-bridged organosilane as a silicon source gives zeolite materials containing an organic group as lattice (ZOL), with several zeolitic phases such as the MFI and the LTA structures. Through various characterization methods, the presence of methylene frameworks (Si-CH2-Si) that replace siloxane bonds (Si-O-Si) has been verified, although the Si-C bonds are partly cleaved to give rise to terminal methyl groups. The shape-selective lipophilicity of a ZOL material indicates that it is not a physical mixture of conventional zeolite and amorphous organic-containing material but contains a genuine organic-inorganic hybrid zeolite.