surfactants and inorganic precursors, it has been possible to create mesoporous materials with different symmetries and pore sizes, and diverse compositions. [5,8] For example, using chiral surfactants as a liquid crystal template has created chiral mesoporous materials with twisted helical structures. [13] In 1999, three research groups independently reported on the incorporation of organic groups into mesoporous silica by using (R′O) 3 SiRSi(OR′) 3 precursors in the place of Si(OR) 4 precursors for the sol-gel condensation. [7,9,14] It proved possible to construct periodic mesoporous silica with organic groups directly integrated into the walls of the mesoporous structure. [11,[15][16][17][18][19][20][21][22][23] Sol-gel processing of silicate materials is highly versatile-it can incorporate various types of precursors and can be carried out under a variety of reaction conditions (e.g., variable pH, temperature, concentration, and solvent mixtures). [24] Therefore, mesoporous organosilica materials have attracted increasing interest for applications including catalysis, [1,25] metal scavenging, [26] chromatography, [27] and biomedical applications. [2] Cellulose nanocrystals (CNCs) obtained from sulfuric-acidcatalyzed hydrolysis of biomass are remarkable materials. [28,29] In 1951, Rånby isolated the crystalline regions within plant cellulose microfibers to form colloidal CNCs with nanoscale dimensions. [28] CNCs have impressive mechanical properties that arise from their high crystallinity and large aspect ratios. [30] Remarkably, CNCs also form a chiral nematic liquid crystal in water. [31] This order can be retained upon drying the aqueous suspension to give a colored, iridescent film. [32] The CNCs arrange into a Bouligand structure, where the crystallites themselves are aligned in layers, but twist with a characteristic helical pitch, P. It is the repeating helicoidal structure that leads to diffraction of circularly polarized light from the CNC films. [33] Many researchers are making new materials that take advantage of the unique properties of CNCs. [30,[34][35][36][37][38][39][40][41][42][43][44][45][46][47] In 2010, we discovered that films of mesoporous silica with chiral nematic structure could be prepared using CNCs as a template. [20] When Si(OR) 4 is condensed with CNCs in water, the resulting composite film contains silica and a chiral nematic assembly of CNCs. CNCs can be removed from the composite materials using pyrolysis, leaving behind thin films of iridescent mesoporous silica with a chiral nematic arrangement of pores inside the glass. These materials are of interest Mesoporous organosilica films with chiral nematic structures are prepared with a bridging urea group and with alkylene bridges, where the length of the alkylene bridge varies from C 1 -C 6 . To synthesize these materials, cellulose nanocrystals (CNCs) are used as liquid crystal templates, which coassemble with the organosilica precursor to give composite materials with a chiral nematic structure of CNCs embedded within. Remova...