Abstract Enhancing fracture toughness and ductility of brittle materials such as concrete remains a challenge. Nature offers numerous mechanisms to enhance fracture toughness using purposeful designs of materials’ architecture. Natural nacre exhibits high fracture toughness by promoting inelastic deformation and hierarchical toughening mechanisms. Here, “nacre‐like‐separated” and “nacre‐like‐grooved” cementitious composites inspired by brick‐and‐mortar arrangement of mollusk shells are proposed. These nacre‐like composites are engineered by laser processing cement paste into individual tablets and grooved patterns (as intentional defects) and laminating them with limited amounts of suitable elastomeric (polyvinyl siloxane) interlayers. It is found that interlayer deformation, tortuous crack propagation guided by the defects, and crack bridging are the main toughening mechanisms in these composites that lead to rising resistance curves. The study hypothesizes tablet sliding as an additional toughening mechanism in “nacre‐like‐separated”, preventing tablet failure and leading to the postponed onset of bulk composite failure. These mechanisms significantly enhance both fracture toughness and ductility by 17.1 and 19 folds, compared to constituent hardened cement paste, respectively. By engineering laser‐induced defects into tabulated cementitious‐elastomeric material at meso‐scale, a class of tough and ductile cementitious composites is introduced, resulting in significantly high fracture toughness values (73.68 MPa.mm 1/2 ), comparable to Ultra‐high‐performance‐concrete without sacrificing the strength.