The present study deals with the processing and characterization of cellulose nanocomposites natural rubber (NR), low-density polyethylene (LDPE) reinforced with carrot nanofibers (CNF) with the semi-interpenetrated network (S-IPN) structure. The nanocomposites were compounded using a co-rotating twin-screw extruder where a master-batch of NR and CNF was fed to the LDPE melt, and the NR phase was crosslinked with dicumyl peroxide. The prepared S-IPN nanocomposites exhibited a significant improvement in tensile modulus and yield strength with 5 wt % CNF content. These improvements are due to a better phase dispersion in the S-IPN nanocomposites compared with the normal blend materials, as demonstrated by optical microscopy, electron microscopy and ultraviolet–visible spectroscopy. The S-IPN nanocomposite also displayed an improved crystallinity and higher thermal resistance compared with NR, CNF, and the normal blend materials.