Novel, tailored titanium dioxide pigments with controllable nanoscale morphological features were shown to significantly enhance the optical and strength properties of paper. The opacifying power of synthesized polycrystalline TiO2 particles in a cellulose matrix was found experimentally to be superior to that of a commercial rutile pigment, depending on the crystal structure of the synthesized particles. High aspect ratio polycrystalline rutile pigments composed of a linear linkage of several individual rutile crystals gave 6% more opacity than the commercial rutile pigment. Theoretical light scattering calculations using the T-Matrix Method showed the light scattering efficiency of linearly arranged polycrystalline rutile particles to depend on number and size of crystals composing the particle and confirmed the higher efficiency of the synthesized polycrystalline rutile pigments over commercial rutile. The opacifying power of hollow polycrystalline rutile particles was found experimentally to be superior to that of a commercial rutile pigment in a highly pressed bleached fiber matrix, depending on cavity size, while the opacifying power of silica-rutile titania core-shell particles was found comparable to commercial rutile at constant titania loading. The light scattering efficiency of titania core-shell particles was shown to be dependant on the light scattering efficiency of the core material. The overall particle shape and aspect ratio of titania core-shell and hollow nanoparticles were shown to be tunable by choosing an appropriate template and coating thickness in layer-by-layer or sol-gel templating synthesis. Inorganic-cellulose core-shell and hollow cellulose nanoparticles were prepared by self-encapsulation with regenerated cellulose via precipitation of cellulose in a polyacrylic acid hydrogel layer surrounding inorganic particle templates in 4-Methylmorpholine N-oxide (NMMO) monohydrate solution. This discrete encapsulation of inorganic pigments with a thin, uniform cellulose shell was found to increase the bondability improvement between the particles and a polysaccharide substrate. The crystallinity of several carbohydrate polymers was shown to significantly affect the bondability of encapsulated core-shell particles.