Designing and controlling particle self-assembly into robust and reliable high-performance smart materials often involves crystalline ordering in curved spaces. Examples include carbon allotropes like graphene, synthetic materials such as colloidosomes, or biological systems like lipid membranes, solid domains on vesicles, or viral capsids. Despite the relevance of these structures, the irreversible deformation and failure of curved crystals is still mostly unexplored. Here, we report simulation results of the mechanical deformation of colloidal crystalline shells that illustrate the subtle role played by geometrically necessary topological defects in controlling plastic yielding and failure. We observe plastic deformation attributable to the migration and reorientation of grain boundary scars, a collective process assisted by the intermittent proliferation of disclination pairs or abrupt structural failure induced by crack nucleating at defects. Our results provide general guiding principles to optimize the structural and mechanical stability of curved colloidal crystals.T he morphology of crystals becomes peculiar when selfassembled on curved shells. For example, the Gaussian curvature of a sphere demands the presence of geometrically necessary rotational defects (disclinations) such as the 12 pentagons in a soccer ball. Disclinations can be found in thin shell structures at different length scales: from the world of carbon allotropes (1) [as in fullerenes, nanotubes, and graphene (2)] to biological systems [such as in lipid membranes (3), solid domains on vesicles (4, 5), or in viral capsids (6-8)], and in synthetic structures such as colloidosomes, colloidal particle shells lying at the interface between two fluids (9-12). Thin-shell structures are often conceived for encapsulation purposes at various scales (i.e., as delivery vehicles of different kinds of cargo, from drugs to flavors and cosmetics) and arise naturally in biological systems. Examples include crystalline and glassy colloidosomes, capsules of Janus and patchy particles, nematic vesicles, and viral capsids.Theoretical considerations indicate that arranging a colloidal crystal into a curved geometry involves elastic deformation and the presence of geometrically necessary disclinations showed by simulations to be attached to extended grain boundary scars (13-15), as also confirmed in several experiments (5,9,16,17). Thus, grain boundary scars are different from standard grain boundaries in that they have a nonzero disclination charge, which makes them more costly. Such a complex topological structure is bound to interfere with the mechanical response of the shell in a way that is still unclear. Understanding this point, however, is of utmost importance to control the deformation of many functionalized self-assembled materials (9,18,19). Numerical and theoretical approaches to date are typically based on solving the elasticity field between grain-boundary scars and deriving equilibrium particle configurations from the effective free energy of the...