There is an increasing interest in developing new technologies enabling the efficient detection and removal of radioactive pollution from seawater. Here, we report a dual-function organic-inorganic mesoporous structure for naked-eye detection and removal of uranyl ions from an aqueous environment. The mesoporous sensor/adsorbent is fabricated via direct template synthesis of highly ordered silica monolith (HOM) starting from a quaternary microemulsion liquid crystalline phase. The produced HOM is subjected to further modifications through growing an organic probe, Omega Chrome Black Blue G (OCBBG), in the cavities and on the outer surface of the silica structure. The spectral response for [HOM-OCBBG→U(VI)] complex shows a maximum reflectance at λmax = 548 nm within 1 min response time (tR); the LOD is close to 9.1 µg/L while the LOQ approaches 30.4 µg/L, this corresponds to the range of concentration where the signal is linear against U(VI) concentration (i.e., 5 to 1000 µg/L) at pH 3.4 with standard deviation(SD) of 0.079 (RSD% = 11.7 at n=10). Experiments and DFT calculations indicate the existence of strong binding energy between the organic probe and uranyl ions forming a complex with blue color that can be detected by naked eyes even at low uranium concentrations. With regard to the radioactive remediation, the new mesoporous sensor/captor is able to reach a maximum capacity of 95 mg/g within a few 2 minutes of the sorption process. The synthesized material can be regenerated using simple leaching and re-used several times without a significant decrease in capacity.