CdTe/CdSe nanocrystal (NC) solar cells with an inverted structure (ITO/ZnO/CdSe/CdTe/Au) have been successfully fabricated by a simple solution process coupled with layer-by-layer sintering techniques. It was found that the device performance is strongly dependent on the annealing strategy, the thickness of the acceptor layer and on the buffer layer of ZnO when the optimal thickness of CdTe is adopted. Without the ZnO buffer layer, a thin film of the CdSeNCs on an ITO substrate shows a rougher morphology, resulting in device shunting. However, when a 40 nm-thick ZnO buffer layer and 60 nm-thick CdSe were employed, the device shows a much higher PCE of 5.81% under device conditions, post-annealing at 340 8C. This value is the highest efficiency ever reported to date for a CdTe/CdSe NC solar cell. Comparing with CdTe/CdSe NC solar cells with the normal device configuration, this device with an inverted structure simultaneously offers good Ohmic contact for carrier collection and efficient harvesting of solar photons in a wide wavelength.