One of the most promising materials for photocatalysis is metal-free graphitic carbon-nitride (g-C3N4) that can be employed for a plethora of purposes, e.g. organic synthesis, energy conversion or wastewater remediation. g-C3N4 contains a suitable band gap in the visible light as well as excellent physicochemical stability. Nevertheless, several challenges have to be tackled with g-C3N4, for example, structural disorder, poor dispersion properties, low conductivity and also inconvenient processing. A combination with polymers belongs to the most versatile strategies to enhance g-C3N4 properties as a way toward advanced materials. The present chapter focuses on the studies and progress in g-C3N4/polymer materials, including (1) photoinitiator properties of g-C3N4, (2) modification of g-C3N4 with polymers for enhanced dispersion, (3) hybrid materials of g-C3N4 and polymers formed by physical or covalent attachment and (4) hydrogels based on g-C3N4. In addition, several applications are highlighted, e.g. biosensors, photocatalysis, batteries, H2 evolution and thin films. At the end, a summary and outlook on future developments as well as current issues of this research area are presented.