Fiber metal laminates (FMLs) have emerged as advanced materials for engineering applications due to their high strength-to-weight ratio. This study aims to understand the mechanical response and failure mechanisms of carbon-fiber reinforced aluminium laminates (CARALL) under monotonic and cyclic loading, specifically uniaxial tensile and low-cycle fatigue (LCF) conditions. CARALL, fabricated with alternating (3/2) layers of AA2024-T3 and unidirectional carbon fiber composite, exhibits superior ultimate tensile strength (UTS) compared to AA2024-T3 sheets, with a distinctive three-zone stress-strain curve. The first zone shows elastic strain in both the aluminium alloy and laminate. The second zone features elastic strain in the laminate and plastic strain in the aluminium alloy. In the third zone, surface modifications enhance adhesion, leading to a sudden load drop due to fiber fracture or delamination. Fractographic analysis indicates no significant necking in the laminate, contrasting with the ductile failure of AA2024-T3. The carbon fiber layer exhibits a pure brittle fracture with visible delamination at the interphase of carbon fiber layer and aluminium alloy sheet. Under LCF conditions, the laminate’s cyclic stress response remains stable, with fatigue cracks initiating in the aluminium layers but mitigated by the carbon fibers, leading to cyclic softening. High-magnification images reveal striation marks and transverse micro-cracks in the aluminium, highlighting the complex interaction between aluminium and carbon fiber layers during fatigue.