Cellulose nanocrystals (CNCs) are excellent candidates for the design and development of multifunctional biomaterials systems to be used in a variety of technologically relevant applications. They may be used as the structural reinforcement phase of polymer matrices, act as catalyst support constituents, as well as drug delivery vectors. Modifying and functionalizing CNCs by introducing specific functional components can impart electronic, magnetic, catalytic, fluorescence and optical properties to the system. In this work we report the successful in situ tethering of iron oxide nanoparticles (IONPs) onto CNCs by the thermal decomposition of Fe(CO) 5 in a H 2 O/DMF suspension. Following this procedure, IONPs consisting of mixtures of Fe 3 O 4 and Fe 2 O 3 with an average diameter of 20 nm were attached to the CNCs. The type of iron oxide species that was generated was determined by selected area electron diffraction (SAED) and energy dispersive spectroscopy (EDS), and the particle size was evaluated by transmission electron microscopy (TEM). Raman spectroscopy was used to characterize the presence and the nature of the molecular interaction between the IONPs and the CNCs.