Inorganic/organic hybrid light-emitting diodes were easily fabricated with a thin film containing water-soluble cadmium selenide nanocrystals and poly(N-vinylcarbazole) as an emitting layer by a spin-coating method. The cadmium selenide nanocrystals were synthesized in aqueous solution with L-cysteine hydrochloride as the stabilizer and were transferred from the aqueous solution into chloroform by a cationic surfactant cetyltrimethyl ammonium bromide. A broad emission spanning the whole visible wavelength range was obtained from the inorganic/organic hybrid devices whether poly(N-vinylcarbazole) was present in the devices or not, and the electroluminescence intensity of the devices increased as the applied voltages increased. However, an obvious blue-shift of the wavelength was observed with the increasing applied voltages in the device with poly(N-vinylcarbazole). Accordingly, the emission color of the device made with poly(N-vinylcarbazole) could be tuned from white to blue by varying the applied voltages, but the emission color of the device made without poly(N-vinylcarbazole) was almost constrained in the white region. This can be attributed to a limited contribution of poly(N-vinylcarbazole) emission to the electroluminescence spectra under the higher applied voltage. By comparing the electroluminescence intensity and the current-voltage characteristics of the devices made with and without poly(N-vinylcarbazole), the performance of the device with poly(N-vinylcarbazole) was improved greatly, which indicated that poly(N-vinylcarbazole) played an important role in the carrier injection and transportation in the device with poly(N-vinylcarbazole).