Lead halide perovskites have been extensively investigated in a host of optoelectronic devices, such as solar cells, light-emitting diodes, and photodetectors. The halogen vacancy defects arising from the halogen-poor growth environment are normally regarded as an unfavorable factor to restrict the device performance. Here, for the first time, we demonstrate the utilization of the vacancy defects in lead halide perovskite nanostructures for achieving high-performance nanofloating gate memories (NFGMs). CH 3 NH 3 PbBr 3 nanocrystals (NCs) were uniformly decorated on the CdS nanoribbon (NR) surface via a facile dip-coating process, forming a CdS NR/CH 3 NH 3 PbBr 3 NC core−shell structure. Significantly, owing to the existence of sufficient carrier trapping states in CH 3 NH 3 PbBr 3 NCs, the hybrid device possessed an ultralarge memory window up to 77.4 V, a long retention time of 12 000 s, a high current ON/OFF ratio of 7 × 10 7 , and a longterm air stability for 50 days. The memory window of the device is among the highest for the low-dimensional nanostructurebased NFGMs. Also, this strategy shows good universality and can be extended to other perovskite nanostructures for the construction of high-performance NFGMs. This work paves the way toward the fabrication of new-generation, high-capacity nonvolatile memories using lead halide perovskite nanostructures. KEYWORDS: nanofloating gate memories (NFGMs), perovskite nanocrystals, CH 3 NH 3 PbBr 3 , CdS nanoribbons (NRs), large memory window