to external stimuli [7] are just a few examples of inspiring features that should be included within synthetic structural materials. They provide inspiration for potential solutions to address challenges associated with traditional approaches of material selection. [8] In the classical approach, a material is selected for a specific application based on the expected loading conditions, design objective and constraints, and databases of material properties with fixed values (e.g., Ashby method [9] ). This methodology does not account for unpredictable loading conditions. To address this issue, safety factors are added, which increases the associated cost and weight of the structure; thus, reduces its mechanical efficiency. A potential solution for this dichotomy is to have materials with adaptable properties responding to loading conditions. This feature can result in materials with improved mechanical efficiency and reduction in costs, resources, and environmental impact. So far, there are few synthetic materials capable of increasing stiffness in response to external stimuli. For example, some investigators have reported polymers that changed elastic moduli by changing the degree of crosslinking upon chemical, thermal, or mechanical stimuli. [10,11] In addition, a study showing an increase of the elastic modulus of liquid crystal elastomers during cyclic Natural structural materials, such as bone, can autonomously modulate their mechanical properties in response to external loading to prevent failure. These material systems smartly control the addition/removal of material in locations of high/low mechanical stress by utilizing local resources guided by biological signals. On the contrary, synthetic structural materials have unchanging mechanical properties limiting their mechanical performance and service life. Inspired by the mineralization process of bone, a material system that adapts its mechanical properties in response to external mechanical loading is reported. It is found that charges from piezoelectric scaffolds can induce mineralization from surrounding media. It is shown that the material system can adapt to external mechanical loading by inducing mineral deposition in proportion to the magnitude of the stress and the resulting piezoelectric charges. Moreover, the mineralization mechanism allows a simple one-step route for fabricating functionally graded materials by controlling the stress distribution along the scaffold. The findings can pave the way for a new class of self-regenerating materials that reinforce regions of high stress or induce deposition of minerals on the damaged areas from the increase in mechanical stress to prevent/mitigate failure. It is envisioned that the findings can contribute to addressing the current challenges of synthetic materials for load-bearing applications from self-adaptive capabilities.The ORCID identification number(s) for the author(s) of this article can be found under https://doi.org/10.1002/adma.201906970.The mechanical efficiency of natural (or biological) s...