Ionogel electrolytes offer excellent ionic conductivity at the expense of mechanical strength because of entrapped electrolytes. Poor mechanical strength coupled with a very low lithium-ion transference number accelerates the lithium dendrite proliferation because of the large polarization gradient. Herein, we propose layer-by-layer (LbL) assembly strategy for simultaneously enhancing mechanical strength, lithium-ion transference number, and electrochemical potential window without affecting ionic conductivity. The essence of our strategy is centered to create the intrinsic ionic structure to reengineer the ionogel membrane’s interfaces. The resulting ultrathin LbL reinforced membrane enhanced the mechanical strength, lithium-ion transference number, and electrochemical potential window, maintaining high ionic conductivity (~ 10^-4 Scm^-1 at 10 °C)¹. The Li|LbL|LFP and Li|LbL|NMC811 full cells exhibit promising electrochemical performances. Comprehensive characterization reveals that LbL membranes enhance the electrochemical performances that will lead to the design of robust electrolyte membranes for high energy density LMBs.