We report a new method for label-free, sensitive, and facile detection of lead(II) ions (Pb 2+ ) based on an aptamer−target binding event, which is recognized by orientations of liquid crystals (LCs) at aqueous interfaces. The LC film suspended in the aqueous phase demonstrated a homeotropic orientation in contact with a cationic surfactant cetyltrimethylammonium bromide (CTAB) due to selfassembly of CTAB molecules at the aqueous−LC interface. The ordering of LC subsequently changed to planar in the presence of the spinach RNA aptamer (SRNA) due to interactions between CTAB and SRNA. In the presence of the Pb 2+ ion, the ordering of LC changed to homeotropic caused by reorganization of CTAB at the LC−aqueous interface. This is due to formation of more stable quadruplex structures of SRNA with Pb 2+ ions in comparison to the CTAB-SRNA complex. The sensor exhibited a detection limit of 3 nM, which is well below the permissible limit of Pb 2+ in drinking water. Our experiments establish that addition of Pb 2+ leads to (i) the formation of Pb 2+ -SRNA complexes and (ii) a decrease in density of SRNA on the LC interface, but additional studies are required to determine which of these processes underlie the response of the LCs to the Pb 2+ . We have also demonstrated the potential application of the LC sensor for detection of Pb 2+ in tap water. Unlike current laboratory-based heavy-metal-ion assays, this method is comparatively simple in terms of instrumentation, operation, and optical readout.