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Novel polyurethane-based binders, specifically designed for environmentally responsible rocket propellant composites, were obtained by employing the polyester-polyols that resulted from the degradation of polyethylene terephthalate waste. A new class of “greener” rocket propellants, comprising polyurethanes (based on recycled PET) as the binder, phase stabilized ammonium nitrate (PSAN) as the eco-friendly oxidizer, and triethylene glycol dinitrate (TEGDN) as the energetic plasticizer, together with aluminum as fuel and Fe₂O₃ as the catalyst, is herein reported. The components of the energetic mixtures were investigated (individually and as composite materials) through specific analytical tools: ¹H-NMR, FT-IR, SEM-EDX, DTA and TGA, tensile and compression tests, DMA, and micro-CT. Moreover, the feasibility of this innovative solution is sustained by the ballistic performances exhibited by these composite materials in a subscale rocket motor, proving that these new formulations are suitable for rocket propellant applications.