Strained carbon nanohoops exhibit attractive photophysical properties due to their unique π-conjugated structure. However, incorporation of such nanohoops into the pincer ligand of metal complexes has rarely been explored. Herein, a new family of highly strained cyclometalated platinum(II) nanohoops has been synthesized and characterized. Strain-promoted C-H bond activation has been observed during the metal coordination process, and Hückel-Möbius topology and random-columnar packing in the solid state are found. Transient absorption spectroscopy revealed the size-dependent excited state properties of the nanohoops. Moreover, the nanohoops have been successfully employed as active materials in the fabrication of solution-processable resistive memory devices, including the use of the smallest platinum(II) nanohoop for the fabrication of a binary memory, with low switching threshold voltages of ca. 1.5 V, high ON/OFF current ratios, and good stability. These results demonstrate that strain incorporation into the structure can be an effective strategy to fundamentally fine-tune the reactivity, optoelectronic, and resistive memory properties.