The extraordinary strength of inner graphene walls in carbon nanotube (CNT) is barely exerted due to the weak inner-wall shear resistance, which extremely limits its load-bearing capability. To overcome such deficiency, nanocarbon architecture engineering from CNT to graphene nanoribbon (GNR) was performed via longitudinal unzipping of multi-walled CNT, which was utilized to reinforce pure Al. Results show that the activation volume of composites at macroyielding point, evaluated by stress relaxation experiments, monotonically decreases from CNT/Al to GNR/Al, which results in the continuous increase of critical resolved shear stress (CRSS) called for dislocation nucleation/cross-slip at the grain boundaries. Shear-lag model and numerical simulations demonstrate the increased load-transfer effect from CNT/Al to GNR/Al. Meanwhile, the isotropic and kinematic hardening in nanocarbon/Al composites were investigated both by loading-unloading-reloading tests and strain hardening model on basis of dislocation behavior, wherein the effective stress was determined as being larger than back stress in the composites. Detailed analysis further indicates that the nanocarbon architecture from CNT to GNR increases the back stress strengthening due to the enhanced dislocation accumulation at nanocarbon/Al interface. Moreover, as CNT was unfolded to GNR, the failure mode of reinforcements in the composites gradually changed from pull-out to breakage.