Transition metals incorporated into polymers lead to unusual or improved physical properties that significantly differ from those of purely organic polymers. A simple and practicable incorporation of diverse transition metals into any available polymer would make an important contribution to overcome some of the synthetic difficulties of metal-polymer hybrid materials. Here, it is demonstrated that atomic layer deposition (ALD) can be a promising means to resolve some of those difficulties. It is found that even polytetrafluoroethylene (PTFE) with its great physical and chemical stability can be easily transformed into a transition metal–PTFE hybrid material simply by applying a metal-oxide ALD process to PTFE. Upon metal incorporation into the PTFE, the molecular structure as well as mechanical properties (tensile behavior) of PTFE were observed to significantly change. For a better understanding of the changes to the material, experimental investigations using Raman spectroscopy, attenuated-total-reflection Fourier-transform infrared spectroscopy, wide-angle X-ray diffraction, and energy-dispersive X-ray analysis were performed. In addition, with density functional theory calculations, potential bonding states of the incorporated metal into PTFE were modeled and predicted. The ALD-based vapor-phase approach for metal incorporation into a polymer could bring about rapid progress in the research area of metal–polymer hybrid materials.