Combining interlocking structures and gradient design, this paper proposes a 2D biomimetic nacreous composite material with a gradient interlocked structure. Experimental and numerical simulation methods are employed to investigate the initiation and propagation behavior of cracks in the regular interlocking and gradient interlocked biomimetic nacreous composite materials. Samples of biomimetic nacreous composite materials with pre-existing cracks are manufactured using 3D printing technology, and uniaxial tensile tests are conducted to explore their crack propagation behavior. For biomimetic nacreous composite materials with periodic interlocking structures, the interlocking angle is found to play an important role in the toughening mechanism of composites. In biomimetic composite materials with large interlocking angles, crack inhibition effects are achieved through structural gradient design, effectively preventing catastrophic failure. Within the numerical analysis framework, a cohesive zone modeling approach is employed to represent the softer phase of the material, and the numerical simulation are validated by direct comparison with experimental results. In addition, a comprehensive numerical analysis is carried out to comprehend how the structural gradient affects the spread of cracks in these nacreous composites. This research not only illuminate the underlying deformation and toughening mechanisms intrinsic to interlocking nacreous composites but also pave the way for innovative strategies in the design of biomimetic materials through the incorporation of structural gradients.