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Cuprous oxide (Cu2O) nano- and microstructures possess unique properties that may find a variety of applications. Environmentally benign synthesis of Cu2O with well-controlled morphology is highly desirable. In this study, Cu2O crystals with tunable shapes are synthesized using cellulose nanofibrils (CNFs) as a shape regulator and the sole reducing agent in aqueous environment. By simply increasing Cu2O precursor concentration, the Cu2O crystals evolved from octahedra to cuboctahedra, and finally cubes, accompanied with increasing size from nano- to microscale. The selection of Cu chelating agent (sodium tartrate or potassium sodium tartrate) affected the crystal growth rate. Transition in the relative intensities of the (111) and the (200) crystalline peaks in their XRD patterns was consistent with the morphology change. During the growth of crystals, CNFs were preferably bound to the {111} crystalline facet. The introduction of KBr to the reaction system produced short hexapods. The resultant CNF-Cu2O hybrids were incorporated into waterborne polyurethane (WPU) films. Even with 0.5 wt% CNF-Cu2O, the WPU film showed significant enhancement in modulus, strength and elongation at break. This work proves the possibility of controlled growth of Cu2O particles aided by CNFs and provides a new strategy for improving the performance of eco-friendly WPU films. [ABSTRACT FROM AUTHOR]