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We develop a computational approach to design 3-D structures that can be fabricated and then assembled and/or actuated by spatially tailoring the layout of multilayer films with eigenstrains. Eigenstrains are stress-free strains when they occur in an unconstrained solid. They are almost an inevitable companion, albeit often unwanted, of thin-film processes. When they vary through the thickness, the constraint of the layers leads to internal stresses and bending and buckling deformations can occur; when they additionally vary in the plane of the film, more complex deformations can result. To advantageously use this phenomenon, we build on relatively simple mechanics ideas in a continuum formulation and combine geometrically nonlinear finite-element analysis of arbitrary-shaped multilayer films with a topology optimization methodology to determine the material layout in each layer so the film deforms into a prescribed shape. We expand our previous experimentally validated approach to include initially curved films and anisotropic eigenstrains. Using an extended system formulation for directly computing instability points allows us to tailor postbuckling response while explicitly controlling the design at limit and bifurcation points. We demonstrate the potential and versatility of our approach by applying it to a series of problems of contemporary and emerging interest.