We report on the development of new 2‐pyridones as an efficient means to avoid the photochemical instability often encountered in organic third‐order nonlinear optical materials. Several push–pull molecules with this particular non‐aromatic heterocycle as a spacer between different donor and acceptor groups have been easily synthesized. The good transmitter behavior of the pyridonic ring is demonstrated and picosecond infrared single‐shot Z‐scan measurements performed in solution show the ability of these molecules to exhibit a stable and off‐resonant optical Kerr effect. A polymer based on this structural design has also been developed.