Simple synthetic modulation based on uranyl acetate and phenanthroline has resulted in two uranyl clusters (1 and 2) with different topologies and nuclearities. Notably, the dimeric complex exhibits distinct luminescence quenching upon UV and X-ray irradiation with detection limits of 4.30 × 10-6 J and 0.32 Gy, respectively. To advance the practical application, 1 was further fabricated with polyvinylidene fluoride into a flexible strip as a UV and X-ray indicator.