A ZnO nanoarchitecture, i.e., ZnO nanosheet (NS) framework, is demonstrated to be a promising electron acceptor and direct electron transport matrix for polymer-inorganic hybrid solar cells. The ZnO NS framework is constructed on nanoneedles/indium tin oxide substrate via a room-temperature chemical bath deposition (RT CBD). The framework morphology can be simply tailored by varying the concentration of precursor solution in the RT CBD. The ZnO nanoarchitecture with an appropriate free space between the NSs is consequently demonstrated to facilitate poly(3-hexylthiophene) (P3HT) infiltration, resulting in superior interface properties, i.e., more efficient charge separation and less charge recombination, in the hybrid. Moreover, apart from the characteristics similar to the ZnO nanorod (NR) array, including vertical feature and single crystalline structure, the ZnO NS framework exhibits a slightly larger absorption edge and a faster electron transport rate. A notable efficiency of 0.88% is therefore attained in the ZnO NS-P3HT hybrid solar cell, which is higher than that of the ZnO NR-P3HT hybrid solar cell.