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Polysilazanes are excellent coating materials, because of their self‐crosslinking in air at low temperatures, high chemical and thermal stability, elevated hardness, and excellent adhesion to many different substrates. Therefore, coatings of two chemically different polysilazanes (crosslinked Durazane 1800 (HTTS)/perhydropolysilazane (PHPS)) are deposited by either dip or spray coating and crosslinked at 200 or 300 °C in air to investigate the chemical composition, surface energy, and coating adhesion in dependency on the precursor type and crosslinking temperature. The silazane HTTS possesses a higher amount of nonpolar organic groups resulting in a lower surface free energy. The anti‐adherence properties are investigated by using a phenolic resin via pull‐off adhesion, which is slightly reduced from 13 MPa for uncoated aluminum to less than 10 MPa for HTTS coated substrates. The addition of different amounts of poly(tetrafluoroethylene) (PTFE) particles causes a remarkable reduction of the surface free energy leading to a strongly reduced pull‐off adhesion of less than 4 MPa of the phenolic resin from the HTTS/PTFE coated substrates. The anti‐adherent properties remain even after repeated pull‐off tests. Because of the excellent properties, the HTTS/PTFE coatings are a very suitable system for easy mold release of plastic parts from metal molds and to replace commercial nonstick PTFE coatings.