Poly(tetrafluoroethylene) (PTFE) sheet was modified with the remote hydrogen plasma, and the effect of the modification on adhesion between the PTFE sheet and copper metal was investigated. The remote hydrogen plasma was able to make PTFE surfaces hydrophilic without etching. In the modification process, defluorination and oxidation occurred on the PTFE surface. Reactivity of defluorination was 25% (estimated from the concentration of CF2 component) -39% (estimated from the F/C atom ratio). Surface modification of PTFE surface by remote hydrogen plasma contributed to the adhesion between PTFE and copper metal. Peel strength was improved from 7.5 to 92 mN/5 mm by surface modification by a factor of 12. Failure of the PTFE/copper adhesive joint occurred at the interface between the PTFE and copper metal layers, rather than in the inner layer of the PTFE polymer or copper metal layers. Remote hydrogen plasma treatment is a preferable pretreatment of PTFE surface for the fabrication of PTFE and copper metal composites.