on poly(p-phenylenevinylene) (PPV) and CdTe nanocrystals (NCs) was developed. [2] This work demonstrated the important influence of hybrid on the performance of solar cells based on aqueous process, encouraging us to further investigate the ASCs with a new configuration.However, the performance of the ASCs is still severely limited by the narrow width of the depletion region, the intrinsic defects of NCs, and the low carrier extraction ability, resulting in low short-circuit current (J sc ) and open voltage (V oc ) as well as a poor fill factor (FF). Many methods including passivating the surface of NCs, [3][4][5] high temperature annealing, [6] designing polymer with novel structure, [2,[7][8][9][10][11] optimizing device architecture, [12][13][14] etc. are developed to address these issues. For example, Wei et al. successfully designed conjugated polymer with high carrier mobility and largely improved device performance. [15] Jin et al. achieved a record PCE of 5.64% (as reported) based on PPV and CdTe NCs by optimizing device structure. [16] However, controlling the width of the depletion region and enhancing carrier extraction ability have been long a challenge.To address these issues, our group further developed an effective strategy that introduced different BHJ structure into the active material. The highest PCE as high as 6.01% was achieved based on ASCs. [17] In that work, one BHJ is consisted of CdTe and TiO 2 NCs and the other is CdTe NCs and PPV. The width of the depletion region and carrier extraction ability were significantly improved compared to previous works. As known, within limits, the thicker the BHJ film is, the better the performance is. In organic solar cells, the BHJ thickness can even reach 210 nm. [18] For aqueous-processed hybrid solar cells (AHSCs), however, the optimum thickness of the CdTe:TiO 2 BHJ film is only ≈30 nm in the double-side bulk heterojunction system mentioned above. In order to increase the BHJ film thickness and form the bicontinueous phase, the content of TiO 2 NCs have to be enhanced because of their small size. However, TiO 2 NCs contribute no photocurrent in the range of visible light and hence further increasing the thickness of BHJ film leads to the decrease of J sc . Although employing TiO 2 NCs with a larger size can obtain a thicker BHJ film and alleviate the decrease of J sc in theory, preparing water-soluble annatase TiO 2 with larger size is difficult and the aggregation occurs during Environmental friendly aqueous-processed solar cells have become one of the most promising candidates for the next-generation photovoltaic devices. Researchers have made lots of progress in designing active materials with novel structures, manipulating the defects in active materials, optimizing device architecture, etc. However, it has long been a challenge to control the width of the depletion region and enhance carrier extraction ability. Fabrication of a thick bulk heterojunction (BHJ) film is an effective strategy to address these issues but difficult to realize. Herein...