This paper reviews the application of self-assembled monolayers (SAMs) of push–pull chromophores in various fields, focusing on their use as active layers and their impact on device performance. SAMs, which are formed by the spontaneous assembly of organic compounds on surfaces, have gained significant attention due to their ability to modify surface properties. Alkanethiols, alkanesilanes, alkanecarboxylates, and alkane-nephosphonates are commonly used in SAMs, while π-conjugated systems, particularly push–pull chromophores, have emerged as important functional components in molecular electronics, bioelectronics, and sensors. Push–pull chromophores, composed of an electron-donating (push) unit and an electron-withdrawing (pull) unit connected by a conjugated bridge, exhibit unique optical and electrical properties. These properties make them valuable for improving the performance of devices such as dye-sensitized solar cells (DSSCs) and perovskite solar cells (PSCs). In DSSCs, push–pull chromophores enhance the absorption spectrum and improve charge separation, leading to higher efficiency. In PSCs, they address issues such as energy band alignment and electron transfer, enhancing device stability. The paper also discusses the use of push–pull chromophores in self-assembled multilayer nanodielectrics (SANDs), which are used in capacitors and gate insulators of organic field-effect transistors (OFETs). The dipole moment of these chromophores, oriented in a specific direction, contributes to the dielectric properties of the layers, making them suitable for high-k dielectric applications. Additionally, the paper explores the electrical and photonic properties generated by ordered assemblies of push–pull chromophores, including high mobility, high crystalline state, superior deep-blue laser characteristics, bistability, and aggregation-induced emission. These properties make push–pull chromophores useful in various optoelectronic devices, such as OLEDs and 2D organic phototransistors. In conclusion, the intrinsic properties of push–pull chromophores, including their donor, acceptor, and spacer characteristics, are crucial for tuning the desired properties in various applications. The careful design of these chromophores through the nature and length of the π-bridge groups, along with the use of different acceptor and donor groups, is essential for optimizing the performance of devices incorporating push–pull chromophores.This paper reviews the application of self-assembled monolayers (SAMs) of push–pull chromophores in various fields, focusing on their use as active layers and their impact on device performance. SAMs, which are formed by the spontaneous assembly of organic compounds on surfaces, have gained significant attention due to their ability to modify surface properties. Alkanethiols, alkanesilanes, alkanecarboxylates, and alkane-nephosphonates are commonly used in SAMs, while π-conjugated systems, particularly push–pull chromophores, have emerged as important functional components in molecular electronics, bioelectronics, and sensors. Push–pull chromophores, composed of an electron-donating (push) unit and an electron-withdrawing (pull) unit connected by a conjugated bridge, exhibit unique optical and electrical properties. These properties make them valuable for improving the performance of devices such as dye-sensitized solar cells (DSSCs) and perovskite solar cells (PSCs). In DSSCs, push–pull chromophores enhance the absorption spectrum and improve charge separation, leading to higher efficiency. In PSCs, they address issues such as energy band alignment and electron transfer, enhancing device stability. The paper also discusses the use of push–pull chromophores in self-assembled multilayer nanodielectrics (SANDs), which are used in capacitors and gate insulators of organic field-effect transistors (OFETs). The dipole moment of these chromophores, oriented in a specific direction, contributes to the dielectric properties of the layers, making them suitable for high-k dielectric applications. Additionally, the paper explores the electrical and photonic properties generated by ordered assemblies of push–pull chromophores, including high mobility, high crystalline state, superior deep-blue laser characteristics, bistability, and aggregation-induced emission. These properties make push–pull chromophores useful in various optoelectronic devices, such as OLEDs and 2D organic phototransistors. In conclusion, the intrinsic properties of push–pull chromophores, including their donor, acceptor, and spacer characteristics, are crucial for tuning the desired properties in various applications. The careful design of these chromophores through the nature and length of the π-bridge groups, along with the use of different acceptor and donor groups, is essential for optimizing the performance of devices incorporating push–pull chromophores.