Hard biological tissues (e.g., nacre and bone) have evolved for millions of years, enabling them to overcome the conflict between different mechanical properties. The key to their success lies in the combination of limited material ingredients (i.e., hard and soft constituents) and mechanistic ingredients (e.g., functional gradients and building block hierarchical organization). However, the contribution of each material and mechanistic ingredient is still unknown, hindering the development of efficient synthetic composites. Quantitative and systematic studies of hard–soft composites are required to unravel every factor's role in properties outcome. Herein, a voxel‐by‐voxel multi‐material 3D printing technique is used to design and additively manufacture different groups of hard–soft composites. Several combinations of gradients, multilevel hierarchies, and brick‐and‐mortar arrangements are created. Single‐edge notched fracture specimens are mechanically tested and computationally simulated using extended finite element method (XFEM). It is found that functional gradients alone are not sufficient to improve fracture properties. However, up to twice the fracture energy of the hard face is observed when combining functional gradients with hierarchical designs, significantly increasing composite properties. Microscopic analysis, digital image correlation, and strain distributions predicted with XFEM are used to discuss the mechanisms responsible for the observed behaviors.@en

The functional gradient is a concept often occurring in nature. This concept can be implemented in the design and fabrication of advanced materials with specific functionalities and properties. Functionally graded materials (FGMs) can effectively eliminate the interface problems in extremely hard–soft connections, and, thus, have numerous and diverse applications in high-tech industries, such as those in biomedical and aerospace fields. Here, using voxel-based multi-material additive manufacturing (AM, = 3D printing) techniques, which works on the basis of material jetting, we studied the fracture behavior of functionally graded soft–hard composites with a pre-existing crack colinear with the gradient direction. We designed, additively manufactured, and mechanically tested the two main types of functionally graded composites, namely, composites with step-wise and continuous gradients. In addition, we changed the length of the transition zone between the hard and soft materials such that it covered 5%, 25%, 50%, or 100% of the width (W) of the specimens. The results showed that except for the fracture strain, the fracture properties of the graded specimens decreased as the length of the transition zone increased. Additionally, it was found that specimens with abrupt hard–soft transitions have significantly better fracture properties than those with continuous gradients. Among the composites with gradients, those with step-wise gradients showed a slightly better fracture resistance compared to those with continuous gradients. In contrast, FGMs with continuous gradients showed higher values of elastic stiffness and fracture energy, which makes each gradient function suitable for different loading scenarios. Moreover, regardless of the gradient function used in the design of the specimens, decreasing the length of the transition zone from 100%W to 5%W increased the fracture resistance of FGMs. We discuss the important underlying fracture mechanisms using data collected from digital image correlation (DIC), digital image microscopy, and scanning electron microscopy (SEM), which were used to analyze the fracture surface.@en