A novel charge-transfer complex film: copper-(n-propyl ester 7,7,8,8-tetracyanoquinodimethane-2,5-ylene-(3-propionic acid))(Cu-TCNQ(C2H4COOC3H7)2) was preparedby spin-coating. Absorption spectra, green-light (514.5 nm) staticrewritable optical recording properties and rewritable mechanism ofthis film were studied. The results show that there are two strongabsorption peaks at 388 nm and 675 nm, which can be assigned toelectronic transitions in anion radicalTCNQ(C2H4COOC3H7)2−.Green-light optical storage experimental results of this filmwere as follows: write-in power was 9 mW, pulse duration was 80 ns;erasing power was 4 mW, pulse duration was 500 ns; the reflectivitycontrast C⩾15%; number of write–erase cycles N⩾100. Itis found that the realization of rewritable optical storage of theCu-TCNQ(C2H4COOC3H7)2 film isrelated to the reversible changes of the optical properties, which iscaused by the reversible charge transfer between copper and n-propylester 7,7,8,8- tetracyanoquinodimethane-2,5-ylene-(3-propionic acid) inthe complex through inducement of laser irradiation.