LAUSR

Asymmetric nanofluidic devices hold great potential in energy conversion applications. However, most of the existing asymmetric nanofluidic devices remain a single‐level asymmetric structure and a single‐ion selective layer, which results in weak ion selectivity and limited energy conversion efficiency. Herein, a multi‐level asymmetric mesoporous carbon/anodized aluminum/mesoporous silica (MC/AAO/MS) nanofluidic device with abundant and ordered mesochannels is constructed from super‐assembly strategy. The resultant MC/AAO/MS exhibits diode‐like ion transport and outstanding ion storage‐release performance. Importantly, MC/AAO/MS couples the MC and MS dual‐ion selective layers, which ensures a high ionic conductance and evidently enhances the cation selectivity. Thereby, the MC/AAO/MS demonstrates ascendant salinity gradient energy conversion performance. The power density and conversion efficiency can reach up to 5.37 W m−2 and 32.79%, respectively. Noteworthy, a good energy conversion performance of 63 mW m−2 can still be achieved upon high working area, outperforming 300% of the performance of MC/AAO and MS/AAO single‐level asymmetric nanochannels. Theoretical calculation further verifies that the multi‐level asymmetric structure and dual‐ion selective transport are the reason for the enhanced cation selectivity and energy conversion efficiency. This work opens a new avenue for constructing multi‐level asymmetric structured nanofluidic devices for various applications.