In this study, we investigate the modulation of energy band in 3D self-assembled nanomembranes containing GaAs/Al0.26Ga0.74As quantum wells (QWs). Photoluminescence (PL) characterizations demonstrate that the self-assembled structures have different optical transition properties and the modulation of the energy band is thus realized. Detailed spectral analyses disclose that the small strain change in structures with different curvatures cannot cause remarkable change in energy bands in Al0.26Ga0.74As layer. On the other hand, the optical transitions of GaAs QW layer is influenced by the strain evolution in term of lightemission intensity. We also find the first order Stark effect in rolled-up nanomembrane with diameter of 150 μm, which is closely connected with the coupling effect between the deformation potential and the piezoelectric potential. Our work may pave a way for the fabrication of high performance rolled-QWinfrared photo-detectors.