Due to increasing public concern over hygiene, there have been many studies investigating antimicrobial and antiviral agents recently. With the aim of developing biobased virucidal/virus capture agents, we report a chemical modification of the cellulose nanocrystals (CNCs) surface with poly(2-dimethylamino) ethyl acrylate) methyl chloride quaternary salt (Q-PDMAEA) to introduce the positively charged functional groups. The surface of CNCs was modified through direct and indirect graft polymerization. Subsequently, the direct and indirect cationization effect on the degree of functionalization, thermal stability, crystallinity, and antiviral activity of CNCs was investigated. Indirect cationization produced the highest degree of polymer grafting, increasing particle size and thermal stability. Further, the modified CNCs were tested for their ability to capture nonenveloped bacteriophages PhiX174 (ΦX174) and MS2. We observed a significant (>4.19 log10) reduction in total viral load by specific functionalized CNCs. However, the activity depended on the structure of functional groups, surface charge density, and the type of virus under study. Overall, the direct and indirect cationization of CNC leads to biobased agents with immobilized cationic charge, with good virus capture activity. Such agents can be used for various applications including textiles, packaging, wastewater treatment, etc.