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Here, we present a novel approach to address this issue by combining MXene (Ti3C2Tx) nanosheets with branched ionic nanoparticles from polyhedral oligomeric silsesquioxanes (POSS) using an amphiphilicity driven assembly for the formation of composite monolayers of nanoparticle-decorated MXene nanosheets at the air-water interface. The amphiphilic hybrid MXene/POSS monolayers allow for the fabrication of organized multilayered films with ionic nanoparticles supporting nanoscale gap between MXene nanosheets. For these composite multilayers we observed a 400% enhancement in specific capacitance compared to pure drop-cast MXene films. Furthermore, dramatically enhanced electrochemical cycling stability for ultrathin film electrodes (< 400 nm in thickness) with a 91% capacitance retention over 10,000 cycles has been achieved. Our results suggest that this insertion of 0D ionic nanoparticles with complementary interactions in-between 2D MXene nanosheets could be extended to other hybrid 0D-2D nanomaterials, providing a promising pathway for the development of hybrid electrode architectures with enhanced ionic transport for long term energy cycling and storage, capacitive deionization, and ionic filtration.