Nanoparticle monolayer sheets are ultrathin inorganic-organic hybrid materials that combine highly controllable optical and electrical properties with mechanical flexibility and remarkable strength. Like other thin sheets, their low bending rigidity allows them to easily roll into or conform to cylindrical geometries. Nanoparticle monolayers not only can bend, but also cope with strain through local particle rearrangement and plastic deformation. This means that, unlike thin sheets such as paper or graphene, nanoparticle sheets can much more easily conform to surfaces with complex topography characterized by non-zero Gaussian curvature, like spherical caps or saddles. Here, we investigate the limits of nanoparticle monolayers' ability to conform to substrates with Gaussian curvature by stamping nanoparticle sheets onto lattices of larger polystyrene spheres. Tuning the local Gaussian curvature by increasing the size of the substrate spheres, we find that the stamped sheet morphology evolves through three characteristic stages: from full substrate coverage, where the sheet extends over the interstices in the lattice, to coverage in the form of caps that conform tightly to the top portion of each sphere and fracture at larger polar angles, to caps that exhibit radial folds. Through analysis of the nanoparticle positions, obtained from scanning electron micrographs, we extract the local strain tensor and track the onset of strain-induced dislocations in the particle arrangement. By considering the interplay of energies for elastic and plastic deformations and adhesion, we construct arguments that capture the observed changes in sheet morphology as Gaussian curvature is tuned over two orders of magnitude.While any flat thin sheet can easily be rolled into a cylinder, common experience suggests that conforming the same sheet to a sphere is considerably more difficult. In order to accommodate the curvature of the sphere, one must fold, cut, or stretch the sheet. On surfaces with Gaussian curvature -that is, curvature in two independent directions, such as on a sphere or saddle -triangles no longer have interior angles which sum to 180 • . Conforming a flat sheet tightly to such a surface thus necessarily introduces stresses from stretching or compression. If the stresses build up, the material may respond by delaminating, forming cracks or dislocations, or forming folds [1,2]. For applications where initially flat sheets are to conform to arbitrary surface topographies, the ability to cope with Gaussian curvature therefore translates into a requirement for high bendability combined with an ability to deform locally in-plane, either elastically or plastically.In close-packed nanoparticle monolayers, individual metallic or semiconducting particle cores are embedded in a matrix of interpenetrating ligand molecules that are attached to each core [3,4]. This organic matrix largely determines the sheet's mechanical properties. While these properties have been studied for sheets in planar geometries [5][6][7] and for cylindri...