Abstract: A growing demand for portable electronics and hybrid/electric vehicles, as well as an expanding global portfolio of intermittent electricity generation sources both highlight the critical need to develop reliable, safe, and efficient energy storage technologies. Recently, our group has been advancing two parallel approaches to form solid electrolyte films based on room temperature ionic liquids (materials known as ionogels)for electrochemical energy storage device applications. The first method utilizes free radical co-polymerization inside an ionic liquid to produce a composite gel, while the second approach employs an acid-catalyzed sol gel reaction network to create an inorganic oxide or polymeric support for the ionic liquid in situ. Ionogels are inherently safer than currently used liquid solvent-based electrolytes due to their nonvolatile, nonflammable and leak-proof nature. Possessing wide windows of electrochemical stability (> 3V), ionogels also enable higher energy density devices. Maintaining a high level of ionic conductivity for fast charging and discharging in supercapacitor structures or batteries within the constraints of minimum gel mechanical integrity can be a key design consideration. In the best-case scenario, ionogels retain nearly identical electrical properties as compared to their constituent neat ionic liquids while providing sufficient flexibility and robustness for intended future applications. Recent findings suggest that controlling ionic liquid—scaffold interactions through rational chemical functionalization of the supporting polymer or inorganic structure is an important strategy by which one can optimize ionogel performance.