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Thermoelectric technology, which is characterized by the interconversion between heat and electricity, is demonstrated as an efficient and environmentally friendly route for thermal energy harvesting and solid-state cooling devices. The pursuit for high-performance room temperature thermoelectric materials is of significant interest. Here, we proposed a design strategy to dramatically improve the thermoelectric response by constructing a hierarchical multiscale conductor network (AgNWs/CNT) in polymer matrix (PEDOT:PSS). At the optimized composition, the highest Seebeck coefficient and electrical conductivity of base treated ternary PEDOT:PSS/AgNWs/CNT composite are optimized to be 58.6 μV K−1 and ∼1950 S cm−1. Correspondingly, the power factor is thus calculated to be on the order of 670 μW m−1 K−2, which is among one of the highest values compared with previous reports. The underlying mechanism is illustrated based on detailed structure, morphology and electron transport quantification. This work affords a novel strategy for the future development of high-performance room temperature nanocomposite thermoelectrics.