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In this paper, we present the synthesis of poly(β‐amino ester)‐based solid polymer electrolytes (SPE) from off‐stoichiometric acrylate‐amine formulations using one‐step, catalyst and solvent free aza‐Michael addition. By varying the monomers, the pendant functionality of the polymer chain structure could be altered. All synthesized polymers yield freestanding and easy to handle electrolyte films and hence are evaluated as a new class of SPEs. The SPE with 1,4‐butanediol diacrylate and propylamine showed the highest conductivity of 1.15 × 10−7 S cm−1 at 30°C with 10 wt% lithium bis(trifluoromethanesulfonyl)imide. Because of the presence of the various functional groups in the structure, the polymer chain aids in the movement of both the anion and the cation. [ABSTRACT FROM AUTHOR]