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Ultrathin flexible encapsulation (UFE) using multilayered films has prospects for practical applications, such as implantable and wearable electronics. However, existing investigations of the effect of mechanical bending strains on electrical properties after the encapsulation procedure provide insufficient information for improving the electrical stability of ultrathin silicon nanomembrane (Si NM)-based metal oxide semiconductor capacitors (MOSCAPs). Here, we used atomic layer deposition and molecular layer deposition to generate 3.5 dyads of alternating 11 nm Al2O3 and 3.5 nm aluminum alkoxide (alucone) nanolaminates on flexible Si NM-based MOSCAPs. Moreover, we bent the MOSCAPs inwardly to radii of 85 and 110.5 mm and outwardly to radii of 77.5 and 38.5 mm. Subsequently, we tested the unbent and bent MOSCAPs to determine the effect of strain on various electrical parameters, namely the maximum capacitance, minimum capacitance, gate leakage current density, hysteresis voltage, effective oxide charge, oxide trapped charge, interface trap density, and frequency dispersion. The comparison of encapsulated and unencapsulated MOSCAPs on these critical parameters at bending strains indicated that Al2O3/alucone nanolaminates stabilized the electrical and interfacial characteristics of the Si NM-based MOSCAPs. These results highlight that ultrathin Al2O3/alucone nanolaminates are promising encapsulation materials for prolonging the operational lifetimes of flexible Si NM-based metal oxide semiconductor field-effect transistors.