A strategy to realize ZnO-based near-white-light electroluminescence (EL) was proposed by utilizing and regulating the intrinsic defect-related emissions of solution-processed ZnO nanocrystals (NCs). Prototype near-white light-emitting diodes (LEDs) based upon this strategy were demonstrated by using n-ZnO NCs/n-Si isotype heterojunctions. The emission color of the n-ZnO NCs/n-Si isotype heterojunction LEDs was tuned toward near white by using an Al-doped ZnO (AZO) spectral "scissor" which can tailor the green light more severely, rather than the blue or red light. Moreover, quantum size effect was clearly observed in both the photoluminescence (PL) and EL spectra via the redshift of the near-band-edge UV emission of the ZnO NCs. The strategy using AZO spectral "scissors" to regulate the VO-related green emission of ZnO may present a promising pathway to realize ZnO-based white-light LEDs.