Laser-induced photoionization and fluorescence signals were simultaneously observed in atomic uranium using a single Nd:YAG-pumped dye laser. These signals were recorded in two specific cases. In the first case, the dye laser was resonant to the first-step transition (0–16900.38cm⁻¹). In the second case, the laser was near-resonant to the first-step transition with a slight detuning (0.15cm⁻¹) so that it became two-photon resonant at 33801.06cm⁻¹. The uranium atoms in the ground state were ionized by a single-color, three-photon photoionization technique resulting in the photoionization signal, and the fluorescence signal was simultaneously obtained from the first excited state involved in the photoionization process. The photoionization and the fluorescence signals in the abovementioned cases were also estimated theoretically for several values of the photoionization cross section for the transition between the second excited state at 33801.06cm⁻¹ and the autoionization state at 50701.59cm⁻¹ using density matrix formalism. From the comparison of theoretically calculated ratios of fluorescence signals in the  two specific cases with the experimentally obtained values, the photoionization cross section for the 33801.06–50701.59cm⁻¹ transition has been obtained, which is found to be (5 ± 1) × 10⁻¹⁶ cm².