chirality-based light emitting diodes (LEDs), [7,8] and so forth. [9,10] Extensive efforts have been applied to a broad range of organic luminophores up till now. [11] However, only a few CPL-active inorganic nanomaterials have been designed recently due to the complexity of fine controlled chiroptical responses and insufficient theoretical background explaining the origin of chirality. [12,13] Various approaches have been developed to realize CPL from inorganic nanomaterials. For instance, nanocrystals could exhibit CPL behaviors through the π conjugated interaction between chiral capping ligand and achiral cores. [12,14] It is also hypothesized that chiral environment could confer CPL on quantum dots (QDs), which has been evidenced by CdS QDs encapsulated in chiral apoferritin. [15] However, these approaches usually need tedious synthesis procedures, and the induced CPL signal is usually very low with the dissymmetry factor only ≈10 −3 -10 −4 . [12][13][14][15][16] Moreover, it is known that most metal-based nanomaterials are toxic and have the disadvantage of high manufacturing cost, which limit their widespread applications. Under this circumstance, it is urgent to develop environmentally friendly and CPL nanomaterials with high strength and capacity for scalable preparations.Silicon-based nanoparticles have gained extensive attentions owing to their desirable properties such as being comprised of earth-abundant elements, favorable biocompatibility, and excellent photostability. [17][18][19] Fluorescent silicon QDs (Si QDs) have been recognized as a promising material sharing remarkable optical and electronic properties of traditional metal-based semiconductor QDs. In the past decades, considerable efforts have been devoted to investigate their synthetic strategies and practical applications. A variety of green and simple synthetic methods have been developed for preparing this promising material. [17,[20][21][22] Besides, the excellent water stability, high fluorescence, and low toxicity make them suitable for applications in plenty of fields such as bioimaging, photocatalysis, and sensing. [23][24][25] Based on these outstanding properties, Si QDs is undoubtedly a prominent candidate for the implementation of CPL. To the best of our knowledge, conferring CPL on Si QDs has not been reported to date.Cellulose nanocrystals (CNCs) are renewable and biocompatible nanomaterials which could be easily obtained from bulk cellulose by acid-hydrolysis. After treating with sulfuric acid, CNCs could exhibit excellent water dispersibility due to negative charge from the enriched sulfonate groups on the surfaces. [26,27] Circularly polarized luminescent inorganics arouses attentions due to scalable preparation and versatile chiral optoelectronic applications. Here, strong circularly polarized luminescence (CPL) activity has been developed from self-assembled cellulose nanocrystals decorated with blue emitting silicon quantum dots (QDs). The electrostatic attraction promotes the successful incorporation of QDs into chiral ...