Upcycling recycled carbon fibers recovered from waste carbon composites can reduce the price of carbon fibers while improving disposal-related environmental problems. This study assessed and characterized recycled carbon fibers subjected to sizing treatment using N-(2-aminoethyl)-3-aminopropyltrimethoxysilane (APS) chemically coordinated with polyamide 6 (PA6) and polypropylene (PP) resins. Sizing treatment with 1 wt.% APS for 10 s yielded O=C-O on the surface of the carbon fiber, and the -SiOH in the APS underwent a dehydration-condensation reaction that converted O=C-O (lactone groups) into bonds of C-O (hydroxyl groups) and C=O (carbonyl groups). The effects of C-O and C=O on the interfacial bonding force increased to a maximum, resulting in an oxygen-to-carbon ratio (O/C) of 0.26. The polar/surface energy ratio showed the highest value of 32.29% at 10 s, and the interfacial bonding force showed the maximum value of 32 MPa at 10 s, which is about 15% better than that of commercial carbon fiber (PA6-based condition). In 10-s resizing treatments with 0.5 wt.% 3-methacryloxypropyltrimethoxysilane (MPS), C-O, C=O, and O=C-O underwent a dehydration-condensation reaction with -SiOH, which broke the bonds between carbon and oxygen and introduced a methacrylate group (H2C=C(CH3)CO2H), resulting in a significant increase in C-O and C=O, with an O/C of 0.51. The polar/surface free energy ratio was about 38% at 10 s, with the interfacial bonding force increasing to 27% compared to commercial carbon fiber (PP-based conditions). The MPS exhibited a superior interfacial shear strength improvement, two times higher than that of APS, with excellent coordination with PP resin and commercial carbon fiber, although the interfacial bonding strength of the PP resin was significantly lower.