Thin films of vinyl derivatives of naphthalene diimide were prepared by electron-assisted vapor deposition. Monomer materials of N, N'-bis(allyl)-naphthalene diimide (Allyl-NDI) and N,N'-bis(p-vinyl-benzyl)-naphthalene diimide (Sty-NDI) were newly synthesized for this purpose. Uniform films were obtained by vapor-depositing these materials, whereas spin-coating yielded nonuniform films. IR analysis suggested that Sty-NDI can be polymerized upon vapor deposition. An insoluble film of Sty-NDI was obtained by the electron-assisted vapor deposition. On the other hand, Allyl-NDI had lower reactivity for polymerization. It was concluded that Sty-NDI is a promising material for preparing thin films of vinyl polymer having naphthalene diimide units.