There is a great demand to develop non-destructive techniques to identify and quantify Special Nuclear Materials (SNM) in homeland security and nuclear safeguards applications. Passive assay could be extremely challenging in some scenarios. Active interrogation technique based on photofission has been identified as one of the promising approaches. In radiation detection system design based on such technique, it is highly desired to have abilities to accurately and efficiently simulate delayed γ-rays emitted from photofission reactions. In this work, simulation results were compared with measurement outcomes to demonstrate the capabilities and limitations of the code MCNPX 2.7.0 in the simulation of delayed γ-rays from photofission of uranium and plutonium samples. First, high-energy delayed γ-rays (Eγ~2.7–4.5MeV) from photofission of 238U were simulated and validated against the energy spectra measured in between linac pulses. Second, low-energy delayed γ-ray spectra (Eγ~0.6–2.7MeV) measured with a list-mode system after irradiation of 239Pu were used in the validation.