Geometric imperfection, known as a detrimental effect on the buckling load of cylindrical shells, has a new role under the emerging trend of using buckling for smart purposes. Eigenshape-based geometries were designed on the shell surface with the aim of tailoring the postbuckling response. Fourteen seeded geometric imperfection (SGI) cylinders were fabricated using polymer-based 3D printing, and their postbuckling responses were numerically simulated with a general-purpose finite element program. Results on the prototyped SGI cylinders showed a tunable elastic postbuckling response in terms of initial and final stiffness, the maximum load drop from mode switching, and the number of snap-buckling events. A response contour and discrete map is presented to show how the number of waves in the axial and circumferential directions in the seeded eigenshape imperfection can control the elastic postbuckling response. SGI cylinders provide diverse design opportunities for controllable unstable response and are good candidates for use in smart and adaptive materials/structures.