In the last few decades, organic materials (or carbon-based materials in a broad sense), including polymers, have received much attention for their potential applications in electronics, because they have outstanding advantages such as high processibility, mechanical flexibility, and low weight. Extensive research efforts have thus been devoted to the development and advancement of organic materials for various applications, covering a wide range from molecular design to device fabrication methods. In addition, it has been recognized that surfaces and interfaces play a crucial role in the operation and performance of the devices. For instance, various interactions at organic-metal interfaces are of great importance in organic epitaxy, and also have a strong correlation with intermolecular structures and their electronic properties. In this context, the main focus of this Special Issue was collecting scientific contributions addressing surface and interface engineering with organic materials, and related applications. The diversity of contributions presented in this Special Issue exhibits relevant progress and the potential of organic materials in a variety of applications that are not limited to the fabrication of organic devices.