The present invention relates to freestanding carbon nanotube paper comprising purified carbon nanotubes, where the purified carbon nanotubes form the freestanding carbon nanotube paper and carbon microparticles embedded in and/or present on a surface of the carbon nanotube paper. The invention also relates to a lithium ion battery, capacitor, supercapacitor, battery/capacitor, and fuel cell containing the freestanding carbon nanotube paper as an electrode. Also disclosed is a method of making a freestanding carbon nanotube paper. This method involves providing purified carbon nanotubes, contacting the purified carbon nanotubes with an organic solvent under conditions effective to form a dispersion comprising the purified carbon nanotubes. The dispersion is formed into a carbon nanotube paper and carbon microparticles are incorporated with the purified carbon nanotubes.