The research work presents a novel methodology to fabricate Al-CNT nanocomposites possessing excellent amalgamation of strength and ductility. A unique combination of processing techniques comprising of ball milling and spark plasma sintering was utilized for consolidating the samples. High-energy ball milling of as-received Al powder and subsequent addition of CNT into the milled Al powder led to a substantial enhancement in the mechanical properties of the resultant composites. Al compact comprising of as-received microcrystalline powder displayed a tensile strength of 105 MPa, which increased to 161 MPa for Al compact with ball-milled nanocrystalline powder. The respective values of ductility reduced from 41.9 to 6.6%. Adding 0.5 wt% CNT in the later compact led to a further upsurge in the tensile strength to 217 MPa; however, the nanocomposite exhibited a further reduction in the ductility to 4.7%. To address this problem, bimodal microstructure was introduced in Al-CNT nanocomposites by using a mixture of nanocrystalline and microcrystalline Al powders (10, 20, 30, 40 and 50 wt%) as the matrix. Al-CNT nanocomposite containing 30 wt% microcrystalline Al powder exhibited a remarkably improved strength-ductility synergy showing 149% higher yield strength and 78% higher tensile strength than the Al compact with microcrystalline grained matrix and 130% higher elongation than the Al-CNT nanocomposite with nanocrystalline grained matrix. Furthermore, to assess the effectiveness of bimodality and CNT reinforcement, experimentally determined value of yield strength of Al-30M70N-CNT was assessed with respect to the theoretically calculated value. It was found that the experimentally obtained yield strength of the nanocomposite was about 94% closer to the predicted value endorsing the effectiveness of the designed fabrication route. [GRAPHICS] .