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Depositing carbon nanotubes (CNTs) into carbon fiber reinforced polymer composites (CFRPs) is challenging because of the need for complicated lab-scale processes and toxic chemical dispersants that makes conventional means of processing less compatible with existing industrial procedures for large-scale applications. In this work, a scalable supercritical CO2-assisted atomization technique is used to effectively deposit hybrid CNTs in CFRPs allowing them to boost their functionality and tailor the microstructure. Cellulose nanocrystals (CNCs) are utilized to create hybrid nanostructures with CNTs (CNC bonded CNT) that enables stabilization of CNTs in nontoxic media, i.e., water, and this promotes the scalability of the process. According to Zeta potential values, CNCs successfully stabilize CNTs in water suspension. Scanning electron microscopy (SEM) micrographs show hybrid CNC bonded CNTs are homogeneously dispersed on the carbon fiber surface. According to the in-situ bending test under the optical microscope, crack propagation is hindered by engineered hybrid CNT nanostructures in the modified CFRP whereas neat CFRP exhibits low crack growth resistance due to the uninterrupted crack propagation in the continuous epoxy matrix. Our results imply that this strategy probes the importance of new controlled manufacturing of hybrid nanostructures through evaporation‑induced self‑assembly of nanocolloidal droplets, and allows for tailoring of the desired properties of nanostructured composites.