We demonstrate reversible and irreversible changes in the ultrafast optical response of multilayer graphene oxide thin films upon electrical and optical stimulus. The reversible effects are due to electrochemical modification of graphene oxide, which allows tuning of the optical response by externally applied bias. Increasing the degree of reduction in graphene oxide causes excited state absorption to gradually switch to saturable absorption for shorter probe wavelengths. Spectral and temporal properties as well as the sign of the ultrafast response can be tuned either by changing the applied bias or exposing to high intensity femtosecond pulses. © 2011 American Institute of Physics.