Zinc oxide was synthesized with ionic liquid tetramethylammonium glycine ([N1111][Gly]) and supramoleculargel N-lauro-L-glutamic acid-di-n-butylamide (GP-1) as co-template by solvothermal method and characterized byX-ray diffraction (XRD), scanning electron microscopy (SEM), transmission electron microscopy (TEM) and UV-visdiffuse reflectance spectrometer. The effects of templating agent dosage and aging time on the morphology, mesoporousstructure, and crystal phase of ZnO were investigated. The results demonstrate that the ionic liquid [N1111][Gly]and GP-1 organogel synergistically control the growth orientation of the crystal, and the morphology of ZnO varies withthe templating agent dosage and aging time. The as-synthesized samples were applied in the catalytic degradation ofCongo red under simulated solar light irradiation. In particular, the synthesized sample (MZ-3-8) with nanosheets morphologyexhibited the best catalytic performance with a degradation rate up to 98% for 90 min, clearly superior to commercialZnO and P-25. Furthermore, the catalyst can be cycled at least eight times with little loss of photocatalytic activity.