Multiphoton dissociation of natural UF6was obtained by simultaneous irradiation with a CF4laser at 615.2 cm−1and a transverse, electric, atmospheric (TEA)‐CO2laser at 1073.3 cm−1using various gas pressures and laser fluences. The dissociation percentagesD235andD238of235UF6and238UF6, 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 ofD235,D238and the resulting enrichment factorF=D235/D238were found from an analysis of the 186‐keV peak, originating in235U, and the 63‐keV peak, originating in234Th, the daughter nucleus of238U. A representative result shows a dissociation of 41±1% and235U enrichment factor of 1.049±0.016 yielded by the excitation of 0.47 Torr gas by 25 laser pulses at 20‐mJ cm−2CF4fluence and 1‐J cm−2CO2fluence.