We have developed a family of selective organic catalysts for ring-opening polymerization reactions.^1,2  In parallel efforts, we have developed new oxidation catalysts² that generate new monomers which were then enchained using organocatalytic polymerization¹ to generate functional materials that proved useful agents for the delivery of messenger RNA into living animals.^4-6 Functional delivery of messenger RNA (mRNA) in-vivo is key to implementing potentially transformative strategies for vaccination, protein replacement therapy and genome editing. The step-economical synthesis and evaluation of a new, tunable and effective class of synthetic biodegradable materials: charge-altering releasable transporters (CARTs) will be described for mRNA delivery. CARTs are structurally unique and operate through an unprecedented mechanism, serving initially as oligo(α-amino ester) cations that complex, protect and deliver mRNA, and then change physical properties through a degradative, charge-neutralizing intramolecular rearrangement, leading to intracellular release of functional mRNA and highly efficient protein expression.