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The possibility to obtain surface layers on water and prepare solid multilayer Langmuir–Blodgett films of medium-density polyethylene is shown. The polymer film on water is stable, demonstrates a reversible surface pressure-area isotherm up to 15 mN/m, and can be deposited onto a substrate using the Langmuir–Blodgett technique in a wide range of surface pressures. The thickness of a single deposited layer is 5.1 nm on average. The dielectric and optical constants of multilayer films are near their bulk values. The films exhibit high dielectric strength of at least 200 MV/m.