With specific fold patterns, a 2D flat origami can be converted into a complex 3D structure under an external driving force. Origami inspires the engineering design of many self-assembled and re-configurable devices. This work aims to apply the level set-based topology optimization to the generative design of origami structures. The origami mechanism is simulated using thin shell models where the deformation on the surface and the deformation in the normal direction can be simplified and well captured. Moreover, the fold pattern is implicitly represented by the boundaries of the level set function. The folding topology is optimized by minimizing a new multiobjective function that balances kinematic performance with structural stiffness and geometric requirements. Besides regular straight folds, our proposed model can mimic crease patterns with curved folds. With the folding curves implicitly represented, the curvature flow is utilized to control the complexity of the folds generated. The performance of the proposed method is demonstrated by the computer generation and physical validation of two thin shell origami designs.