Chemically cross-linked cellulose nanocrystal aerogels represent a versatile and universal substrate on which to prepare lightweight hybrid materials. In situ incorporation of polypyrrole nanofibers, polypyrrole-coated carbon nanotubes, and manganese dioxide nanoparticles in the aerogels gives flexible 3D supercapacitor devices with excellent capacitance retention, low internal resistance, and fast charge-discharge rates.