The present work introduces a comparative study on the use of polymer nanocomposites containing clay minerals of different structure, such as montmorillonite and sepiolite as host solids for the templating synthesis of carbon-like materials from different organic precursors. Carbon-clay nanocomposites were obtained by polymerization of either acrylonitrile or sucrose previously inserted in the pores of the clay minerals, followed by their further thermal transformation in carbon-like compounds. Acid treatment of the resulting carbon-clay nanocomposites removes the inorganic templates giving carbon-like materials with different textural features. Polymer-clay, carbon-clay and carbon-like materials have been characterized by applying spectroscopic techniques as FTIR and in situ EIS (electrochemical impedance spectroscopy) and other structural, textural and analytical tools (chemical analysis, XRD, SEM-EDX, TEM-EDX, N2 adsorption isotherms,...). Electrochemical properties of these carbon-clay nanocomposites, as well as their templated carbonaceous materials and their use as electrode materials of different electrochemical devices such as rechargeable Li-batteries, supercapacitors and electrochemical sensors, are also discussed.