Lithium-ion batteries (LIBs) for electric vehicles are facing challenges of unsatisfied volumetric/gravimetric energy densities and the safety issue. Metallization of polyethylene terephthalate (PET) using Cu coatings to form hybrid anode current collectors is a promising strategy to simultaneously address the abovementioned energy density and safety issues. Electrodeposition of Cu on PET is a common method for rapid fabrication of PET-Cu current collectors, showing advantages of high efficiency and low cost. However, the interaction between PET and electrodeposited Cu is usually weak. In this study, a single-wall carbon nanotube (SWCNT) film is introduced at the PET-Cu interface to interlock PET with Cu due to its unique physiochemical properties and network structure. In consequence, improved interfacial adhesion was obtained by electrodepositing Cu on the SWCNT-covered PET (ECu/SWCNT/PET), where the interfacial adhesion strength was improved by 1.57 times. The pouch cell assembled using ECu/SWCNT/PET current collector maintained 97.3% of the initial capacity after 430 cycles, which is comparable to that using a pure Cu current collector. Furthermore, ECu/SWCNT/PET current collector showed advantage in maintaining stability of output voltage during nail penetration test. The ECu/CNT/PET is expected to be used as anode current collector in future lightweight and high-safety LIBs.