The aim of this study was to observe the atmospheric pressure plasma for polytetrafluoroethylene (PTFE) surface modification. The hydrophilicity of the effectively-anchored acrylic acid polymerization on the PTFE surfaces through atmospheric pressure plasma-grafted polymerization was examined using surface chemical composition analysis. The hydrophilic acrylic acid coating was created, via graft polymerization, onto a PTFE surface that was activated by the atmospheric pressure plasma. The photoemission plasma species in this plasma were identified by optical emission spectroscopy. The influences of atmospheric pressure plasma on the PTFE surface properties were also studied. We observed a significant increase in the surface free energy of the PTFE due to the atmospheric pressure plasma treatments. In this study, the changes in the chemical composition of this plasma-grafted, polymerized PTFE surfaces were also determined using FTIR, ESR, and XPS. It suggests that a specific level of surface wettability can be attained by tailor-designing the characteristics of the atmospheric pressure plasma-grafted, acrylic acid polymerization on the PTFE surface by adjusting the chemical composition and surface morphology, which are organized by the plasma surface activation and monomer concentration.