We demonstrate a simple approach to generate phase segregation between colloidal PbS nanocrystals (NCs) and organic [6,6]-phenyl C61 butyric acid methyl ester (PC61BM). Continuous vertical phase segregation is observed in cross-linked composite films of NCs and PC61BM. Hybrid bulk heterojunction photovoltaic cells fabricated with the phase segreated composite layer have achieved the state-of-art power conversion efficiency of 3.7% under one sun of simulated Air Mass 1.5 Global solar irradiation. The presented method can be generally applied in other NC/organic systems for the development of hybrid heterojunction photovoltaic cells.

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