exploited for the purpose of uniform backlighting, brightness enhancement, efficiency improvement, and increased sensitivity in liquid crystal displays (LCDs), [1][2][3] light-emitting diodes (LEDs), [4][5][6] solar cells, [7][8][9] and photodetectors, [10][11][12] all via excellent light scattering properties of optical diffusers.As a nontoxic and biodegradable material, cellulose nanocrystals (CNCs) are environment friendly. They are directly extracted from natural resources such as wood and other fiber supplies available in plants. As a high-molecular-weight linear polymer formed of monomers linked together by glycosidic oxygen bridges, [13] they offer desirable bulk and nanoscale properties (e.g., high tensile strength, high surface area for interaction with surrounding species) [14] that make them suited for use as substrates in devices such as sensors, [15] solar cells, [16] LEDs, [17] and transistors. [18] In addition, recently, cellulose nanofiber (CNF)-based films and papers have attracted attention for their light scattering capabilities. [9,19,20] Both CNCs and CNFs are very similar in terms of chemical composition and can be derived from the same source but are morphologically different in that CNFs are long (in order of micrometers) and flexible composed of both crystalline and amorphous parts while CNCs are short rod-like crystals with lengths in the range of a few hundreds of nanometers. [21] Here, we propose, fabricate, and characterize a new class of optical diffusers based on CNP hybrid films. While some of the recently proposed volumetric diffusers are made of rare earth materials such as cerium [22] which can drive up the cost of fabrication, the proposed diffuser relies on a ubiquitous and environment-friendly material, cellulose, which is cost-effective to produce. Our hybrid diffuser achieves high haze values (up to 85%), which is significantly higher than cellulose nanofiber/ wood pulp diffusers, [9,20] while maintaining a high degree of transparency (≈85%). In addition, unlike previously reported cellulose nanofiber/wood pulp optical diffusers which require an additional index-matching layer between the diffuser and the device for efficient light coupling, [9,20] no index-matching is required for the diffuser here due to the hydrophobic surfaces A novel optical diffuser based on cellulose nanocrystals (CNCs) embedded in polydimethylsiloxane (PDMS) matrix, or cellulose nanocrystal:polymer (CNP) is reported. By offering simple low-cost fabrication process as well as compatibility with large-scale production, the proposed optical diffuser is a better choice for integration into optoelectronic devices for light management compared to other cellulose-based diffusers due to its physical durability and the lack of requirement for index-matching between the diffuser and the optoelectronic device thanks to the unique surface properties, mechanical flexibility, and optical transparency offered by PDMS as the matrix material. It is demonstrated that CNCs are an excellent filler material to pair up w...