Photoinduced electron transfer in molecular hetero- Langmuir-Blodgett (LB) films consisting of Green fluorescent protein (GFP)/viologe/TCNQ was investigated. in this work, charge transfer process in the molecular hetero-films has been investigated by femto-second transient absorption spectroscopy. Based on the transient absorption in the GFP/viologen/TCNQ series hetero-films. charge transfer from excited GFP to viologen (TCNQ) was observed with subpicosecond time resolution.