Overcoming Challenges in Small‐Ring Transfer: Direct Decarboxylative Hydroalkylation of Alkenes via Iron‐Thiol Catalysis

-containing cyclopropyl and cyclobutyl radicals. Synergistic experimental, spectroscopic, and density functional theory (DFT) studies support the proposed reaction mechanism. Additionally, we employed the radical stabilization energy (RSE) scale, developed using isodesmic equations computed at the DFT level, aiming to provide a better understanding of the reluctant radical decarboxylation of small-strained cycloalkanes.