The application of a gel polymer electrolyte (GPE) in electrochemical devices such as batteries, electrochemical double layer capacitors (EDLCs), and others is a known topic in the literature. However, GPE with improved ionic conductivity and better mechanical properties are highly desired. In this work, ionogel polymer electrolytes (IGPEs) were synthesized by photopolymerization of a mixture of monomers: aliphatic urethane diacrylate, 1,3,5-triallyl-1,3,5-triazine-2,4,6(1H,3H,5H)-trione, trimethylolpropane triacrylate, pentaerythritol tetrakis(3-mercaptopropionate) in 1-ethyl-3-methylimidazolium bis(trifluorometh-ylsulfonyl)imide (EMImNTf 2 ). The influence of the monomer ratio on the ionic conductivity and mechanical properties of IGPEs was studied. A mathematical model was used to optimize the composition to obtain ionogel with the best compromise between investigated properties. The optimal composition was synthesized and used in EDLC, characterized by higher volumetric capacity, power, and energy density. To the best of our knowledge, this is the first publication that demonstrates the application of optimization methods for the preparation of IGPEs.