In an effort to create a paintable/printable thermoelectric material, comprised exclusively of organic components, polyaniline (PANi), graphene, and double-walled carbon nanotubes (DWNT) were alternately deposited from aqueous solutions using the layer-by-layer assembly technique. Graphene and DWNT are stabilized with an intrinsically conductive polymer, poly(3,4-ethylenedioxythiophene):poly(styrenesulfonate) (PEDOT:PSS). A 1 µm thick film, composed of 80 PANi/graphene-PEDOT:PSS/PANi/DWNT-PEDOT:PSS quadlayers (QL) exhibits electrical conductivity (σ) of 1.88 X 10⁵ S/m and a Seebeck coefficient (S) of 120 µV/K, producing a thermoelectric power factor (S²∙σ) of 2710 µW/(m∙K²). This is the highest value ever reported for a completely organic material measured at room temperature. Furthermore, this performance matches or exceeds that of commercial bismuth telluride. These outstanding properties are attributed to the highly ordered structure in the multilayer assembly. The thermoelectric power output increased with the number of cycles deposited, yielding 8.5 nW at 80 QL for ΔT = 5.6 K. A simple thermoelectric generator was prepared with selectively-patterned, fabric-based system. The electric voltage generated by each TE device increased in a linear relationship with both ΔT and the number of TE legs, producing ~ 5 mV with just five legs and a ΔT of 9.5 K. This unique TE coating system is water-based and uses only organic components. For the first time, there is a real opportunity to harness waste heat from unconventional sources, such as body heat to power devices in an environmentally-benign way.