In ferroelectrets, the piezoelectricity stems from the charges of both polarities trapped on the inner surfaces of the cavities in the material, so that its thermal stability is defined by the stability of the respective charges. In the present work, a template-based lamination technique has been employed to fabricate tubular-channel ferroelectrets from fluoroethylenepropylene (FEP) films. It has been shown that the piezoelectricity in FEP ferroelectrets decays at relatively low temperatures due to the inherently lower thermal stability of the positive charge. In order to improve charge trapping, we have treated both FEP films and inner surfaces of the ferroelectret cavities with titanium-tetrachloride vapor, using the atomic-layer-deposition technique. Using surface-potential-decay measurements on FEP films, we have found that the charge-decay curves shift by more than 100 °C to the higher temperatures as a result of the surface treatment. Direct measurements of piezoelectric d33 coefficients as a function of temperature have shown that the piezoelectric stability is likewise improved with the d33-decay curves shifted by 60 °C to the right. The improvement of electret/ferroelectret properties can be attributed to the formation of the deeper traps on the chemically modified FEP surface. SEM micrographs and EDS analysis reveal island-like structures with titanium- and oxygen-containing species that can be responsible for the deeper trapping of the electret charges.