The cover picture shows the molecular building block, which plays the major role in this type of material. The organically functionalized spherosilicate contains furanyl groups at all eight corners, which act as dienes in the Diels–Alder reaction. The synthesis of this inorganic building block is straightforward and it can be achieved easily in a multigram scale. The scheme below shows the principle of the crosslinking and de‐crosslinking reaction in the material, which is a prerequisite for the self‐healing cycles. In the background, a macroscopic self‐healing process is shown by the disappearance of surface scratches, which is also presented in the paper. Details are discussed in the article by T. Engel and G. Kickelbick on p. 1226 ff. For more on the story behind the cover research, see the Cover Profile.