Solution-processed organic-inorganic hybrids composing of MoO3 nanoparticles and PEDOT:PSS were developed for use in inverted organic solar cells as hole transporting layer (HTL). The hybrid MoO3:PEDOT:PSS inks were prepared by simply mixing PEDOT:PSS aqueous and MoO3 ethanol suspension together. A core-shell structure was proposed in the MoO3:PEDOT:PSS hybrid ink, where PEDOT chains act as the core and MoO3 nanoparticles connected with PSS chains act as the composite shell. The mixing with PEDOT:PSS suppressed the aggregation of MoO3 nanoparticles, which led to a smoother surface. In addition, since the hydrophilic PSS chains were passivated through preferentially connection with MoO3, the stronger adhesion between MoO3 nanoparticles and the photoactive layer improved the film forming ability of the MoO3:PEDOT:PSS hybrid ink. The MoO3:PEDOT:PSS hybrid HTL can therefore be feasibly deposited onto the hydrophobic photoactive polymer layer without any surface treatment. The use of the MoO3:PEDOT:PSS hybrid HTL resulted in the optimized P3HT:PC61BM- and PTB7:PC61BM-based inverted organic solar cells reaching highest power conversion efficiencies of 3.29% and 5.92%, respectively, which were comparable with that of the control devices using thermally evaporated MoO3 HTL (3.05% and 6.01%, respectively). Furthermore, less HTL thickness dependence of device performance was found for the hybrid HTL-based devices, which makes it more compatible with roll-to-roll printing process. In the end, influence of the blend ratio of MoO3 to PEDOT:PSS on photovoltaic performance and device stability was studied carefully, results indicated that the device performance would decrease with the increase of MoO3 blended ratio, whereas the long-term stability was improved.