<jats:p>Organic materials have attracted considerable attention for thermoelectric (TE) applications. Given their potential as wearable power generators, there is an urgent need to develop organic TE materials that possess superior electronic properties as well as excellent mechanical and environmental stability. Here, we develop paper-based TE materials using the poly(3,4-ethylenedioxythiophene): polystyrenesulfonate (PEDOT:PSS), graphene nanoplatelets (GNPs), and a starch-based biopolymer as a binder for GNPs. The device fabrication consists of spraying the biopolymer/GNP ink onto the cellulose paper followed by spraying the PEDOT:PSS solution. Further enhancement of TE properties was obtained by adding an ionic liquid (IL), bis(trifluoromethane)sulfonimide lithium salt to the PEDOT:PSS solution. Upon addition of the IL, the electrical conductivity of as-fabricated PEDOT:PSS films increased nearly two orders of magnitude. The electrical conductivity increases with GNPs' content due to formation of an effective electrical percolation network. Interestingly, incorporating GNPs simultaneously improves the Seebeck coefficient. Raman measurements suggest that the concurrent enhancement of the Seebeck coefficient and electrical conductivity might be related to the chemical bonding between the conducting polymer chains and the filler. In addition, these composites display remarkable flexibility at various bending angles and environmental stability without losing their original conductivity after three months of exposure to ambient conditions.</jats:p>