Interface enhancement with carbon nanotubes (CNTs) provides a promising approach for improving shock strength and toughness of glass fiber reinforced plastic (GFRP) composites. The effects of incorporating flame-synthesized CNTs (F-CNTs) into GFRP were studied, including on hand lay-up preparation, microstructural characterization, mechanical properties, fracture morphologies, and theoretical calculation. The experimental results showed that: (1) the impact strength of the GFRP modified by F-CNTs increased by more than 15% over that of the GFRP modified by CNTs from chemical vapor deposition; and (2) with the F-CNT enhancement, no interfacial debonding was observed at the interface between the fiber and resin matrix on the GFRP fracture surface, which indicated strong adhesive strength between them. The theoretical calculation revealed that the intrinsic characteristics of the F-CNTs, including lower crystallinity with a large number of defects and chemical functional groups on the surface, promoted their surface activity and dispersibility at the interface, which improved the interfacial bond strength of GFRP.