Al-doped ZnO nanoparticles were synthesized using the green method for dye degradation activity for the first time. The Allium Calocephalum Wendelbow (ACW) plant leaf extract has been employed in the biosynthesis of the aluminum (Al) doped and undoped (pure) zinc oxide (ZnO) nanoparticles (NPs) for the applicability of dye degradation capability. In order to investigate the dye degradation behavior process, methylene orange (MO) is being used. For produced Al-doped and undoped ZnO NPs, the efficiency and sustainability of the (ACW) leaf plant for the dye decomposition process has been examined. The produced Al-doped and pure ZnO NPs have been studied for their quality and structure using a variety of characterization technique. For the first time, the green synthesis process was applied in order to thoroughly examine the impact of the various Al-doped green ZnO nanoparticle ratios on the average size, shape, distribution, crystal structure, functional group, optical capabilities, chemical compositions, and energy band-gap. The ratio of Al-doped ZnO NPs consisted of 0% (pure), 0.025%, 0.050%, 0.075%, 0.10%, and 0.20%. The results demonstrate that the characteristics of the doped and pure green ZnO NPs are significantly affected by the varied Al-doped ZnO ratio. ACW plant leaf extract was examined using FTIR and UV–Visible spectroscopy, and the results suggested that this extract might be a promising alternative for the environmentally friendly synthesizing of both doped and undoped ZnO NPs. At ambient temperature, the UV–Visible spectra of leaf extract displayed two separate absorption peaks roughly at 262 nm and 350 nm. As additional proof of the ACW plant's use of the green method in this research, the examination of the MO dye degrading activity by Al-doped and pure ZnO NPs was conducted utilizing the newly produced Al-doped and pure ZnO NPs made to utilize the green technology. The Al-doped ZnO NPs produced at a ratio of 0.075% displayed a significant degradation rate percentage when dye degradation ability was measured with UV light. Also, the average dye degradation percentage of 90.5% for 80 min of the fabricated Al-doped green ZnO NPs displayed a quicker than average dye degradation percentage of 74% for 140 min of the fabricated pure green ZnO NPs.