Nanocellulose, which can be derived from any cellulosic biomass, has emerged as an appealing nanoscale scaffold to develop inorganic-organic nanocomposites for a wide range of applications. In this study, titanium dioxide (TiO2) nanocrystals were synthesized in the cellulose nanocrystal (CNC) scaffold using a simple approach, i.e., hydrolysis of a titanium oxysulfate precursor in a CNC suspension at low temperature. The resulting TiO2 nanoparticles exhibited a narrow size range between 3 and 5 nm, uniformly distributed on and strongly adhered to the CNC surface. The structure of the resulting nanocomposite was evaluated by transmission electron microscopy (TEM) and X-ray diffraction (XRD) methods. The growth mechanism of TiO2 nanocrystals in the CNC scaffold was also investigated by solution small-angle X-ray scattering (SAXS), where the results suggested the mineralization process could be described by the Lifshitz-Slyozov-Wagner theory for Ostwald ripening. The demonstrated TiO2/CNC nanocomposite system exhibited excellent performance in dye degradation and antibacterial activity, suitable for a wide range of environmental remediation applications.