Traditionally, electrochromic materials rely on counter redox materials like ferrocene to realize redox processes. In this work, two novel, closely related series of electrochromic materials bearing push‐pull electronic structure were designed and synthesised (N,N,N',N'‐tetra(pyridin‐4‐yl)‐1,4‐phenylenediamine derivatives (TPPDs) and N,N,N′,N′‐tetra(pyridin‐4‐yl)benzidine derivatives (TPBDs)). When stimulated by an external electric field, both series of compounds exhibited intramolecular charge transfer because of their push‐pull electronic structures. Therefore, the TPPDs and TPBDs could undergo redox processes without the assistance of counter electrode chemicals. Furthermore, the TPPDs and TPBDs could replace the electrolyte that is required in conventional electrochromic devices (ECDs) because of their conductivity. This allowed the fabrication of a simple, single‐component ECD. [ABSTRACT FROM AUTHOR]