We have investigated the effects of two different strain-relief bilayer shell structures on the luminescent properties of colloidal CdSe quantum dots (QDs). CdSe QDs with a strain-compensated ZnS/ZnCdS bilayer shell were synthesized using the successive ion layer adsorption and reaction technique and their crystallinity of was examined by X-ray diffraction. The QDs enjoyed the benefits of excellent exciton confinement by the ZnS intermediate shell and strain compensation by the ZnCdS outer shell. The resulting CdSe/ZnS/ZnCdS QDs exhibited 40% stronger photoluminescence and a smaller peak redshift upon shell growth compared to conventional CdSe/ZnCdS/ZnS core/shell/shell QDs with an intermediate lattice adaptor. CdSe/ZnS/ZnCdS QD light-emitting diodes (LEDs) had a luminance of 558 cd/m2 at 20 mA/cm2, 28% higher than that of CdSe/ZnCdS/ZnS QD-LEDs. The former also had better spectral purity. These results suggest that nanocrystal shells may be strain-engineered in a different way to achieve QDs of high crystalline and optical quality well suited for full-color display applications.