Multiphoton dissociation of natural UF6 was obtained by simultaneous irradiation with a CF4 laser at 615.2 cm−1 and a transverse, electric, atmospheric (TEA)‐CO2 laser at 1073.3 cm−1 using various gas pressures and laser fluences. The dissociation percentages D235 and D238 of 235UF6 and 238UF6, respectively, were determined by comparing results of an irradiated sample to those of a nonirradiated reference sample prepared under identical conditions. For the analysis we employed a simple, high‐precision nuclear technique based on gamma‐ray spectrometry. The values of D235,D238 and the resulting enrichment factor F = D235/D238 were found from an analysis of the 186‐keV peak, originating in 235U, and the 63‐keV peak, originating in 234Th, the daughter nucleus of 238U. A representative result shows a dissociation of 41±1% and 235U enrichment factor of 1.049±0.016 yielded by the excitation of 0.47 Torr gas by 25 laser pulses at 20‐mJ cm−2 CF4 fluence and 1‐J cm−2 CO2 fluence.