Regenerated cellulose fibers coated with copper via electroless plating process are investigated for their mechanical properties, molecular structure changes, and suitability for use in sensing applications. Mechanical properties are evaluated in terms of tensile stiffness and strength of fiber tows before, during and after the plating process. The effect of the treatment on the molecular structure of fibers is investigated by measuring their thermal stability with differential scanning calorimetry and obtaining Raman spectra of fibers at different stages of the treatment. Results show that the last stage in the electroless process (the plating step) is the most detrimental, causing changes in fibers’ properties. Fibers seem to lose their structural integrity and develop surface defects that result in a substantial loss in their mechanical strength. However, repeating the process more than once or elongating the residence time in the plating bath does not show a further negative effect on the strength but contributes to the increase in the copper coating thickness, and, subsequently, the final stiffness of the tows. Monitoring the changes in resistance values with applied strain on a model composite made of these conductive tows show an excellent correlation between the increase in strain and increase in electrical resistance. These results indicate that these fibers show potential when combined with conventional composites of glass or carbon fibers as structure monitoring devices without largely affecting their mechanical performance.