Ferroelectrets have been fabricated from low-density polyethylene (LDPE) films by means of a template-based lamination. The temperature dependence of the piezoelectric d33 coefficient has been investigated. It was found that low-density polyethylene ferroelectrets have rather low thermal stability with the piezoelectric coefficient decaying almost to zero already at 100 °C. This behavior is attributed to the poor electret properties of the polyethylene films used for the fabrication of the ferroelectrets. In order to improve the charge trapping and the thermal stability of electret charge and piezoelectricity, LDPE ferroelectrets were treated with orthophosphoric acid. The treatment resulted in considerable improvements of the charge stability in LDPE films and in ferroelectret systems made from them. For example, the charge and piezoelectric-coefficient decay curves shifted to higher temperatures by 60 K and 40 K, respectively. It is shown that the decay of the piezoelectric coefficient in LDPE ferroelectrets is governed by the relaxation of less stable positive charges. The treatment also leads to noticeable changes in the chemical composition of the LDPE surface. Infrared spectroscopy reveals absorption bands attributed to phosphorus-containing structures, while scanning electron microscopy shows new island-like structures, 50–200 nm in diameter, on the modified surface.