Core–shell nanogels are attractive stabilizers and supports for catalytically active metallic nanoparticles. Herein, we present the synthesis and the characterization of a nanostructured well‐defined core–shell nanogel with the ability to stabilize Pd0 nanoparticles in its core. This hybrid nanogel displays a remarkable stability in both the solid state and in solution. This feature allowed its successful application as a catalyst for the Mizoroki–Heck reaction between n‐butyl acrylate and a series of bromo‐ and iodoarenes. The yields spanned from good to excellent, and catalyst recycling could be achieved up to three times without a significant activity loss. Three‐phase tests indicated that the hybrid nanogel acts as a Pd0 nanoreservoir. The catalysis proceeds in a quasihomogeneous fashion as part of the catalytic activity occurs outside the nanogel, which explains the observed limited recyclability.

An organogel is obtained when a low molar mass compound forms a network of anisotropic fibres in a liquid that is therefore transformed into a macroscopic solid. Various approaches have been proposed to correlate organogel formation and Hansen solubility parameters. These approaches are well adapted to specific experimental datasets but lack universality. A general method to determine the gelation domain from the solubility data of low molecular weight gelators is here reported.