We demonstrate how programmable shape evolution and deformation can be induced in plant-based natural materials through standard digital printing technologies. With nonallergenic pollen paper as the substrate material, we show how specific geometrical features and architectures can be custom designed through digital printing of patterns to modulate hygrophobicity, geometry, and complex shapes. These autonomously hygromorphing configurations can be "frozen" by postprocessing coatings to meet the needs of a wide spectrum of uses and applications. Through computational simulations involving the finite element method and accompanying experiments, we develop quantitative insights and a general framework for creating complex shapes in eco-friendly natural materials with potential sustainable applications for scalable manufacturing., Competing Interests: Competing interest statement: Z.Z., S.S., and N.-J.C. are listed as coinventors on a technology disclosure that was filed in relation to the findings of this study., (Copyright © 2021 the Author(s). Published by PNAS.)