In this study, Al, Zn, Mg and Cu elemental metal powders were chosen as the raw powders. The nanocrystalline Al-7Zn-2.5Mg-2.5Cu bulk alloy was prepared by mechanical alloying and spark plasma sintering. The effect of milling time on the morphology and crystal structure was investigated, as well as the microstructure and mechanical properties of the sintered samples. The results show that Zn, Mg and Cu alloy elements gradually dissolved in α-Al with the extension of ball milling time. The morphology of the ball-milled Al powder exhibited flaking, crushing and welding. When the ball milling time was 30 h, the powder particle size was 2–5 μm. The α-Al grain size was 23.2 nm. The lattice distortion was 0.156% causing by the solid solution of the metal atoms. The grain size of ball-milled powder grew during the spark plasma sintering process. The grain size of α-Al increased from 23.2 nm in the powder to 53.5 nm in the sintered sample during the sintering process after 30 h of ball milling. At the same time, the bulk alloy precipitated micron-sized Al2Cu and nano-sized MgZn2 in the α-Al crystal. With the extension of ball milling time, the compression strength, yield strength and Vickers hardness of spark plasma sintering (SPS) samples increased, while the engineering strain decreased. The compression strength, engineering strain and Vickers hardness of sintered samples prepared by 30 h milled powder were ~908 MPa, ~8.1% and ~235 HV, respectively. The high strength of the nanocrystalline Al-7Zn-2.5Mg-2.5Cu bulk alloy was attributed to fine-grained strengthening, dislocation strengthening and Orowan strengthening due to the precipitated second phase particles.