Carbon in its elemental state has a long tradition as filler for polymers. Already in the First Dynasty of Egypt (3100-3050 B.C.) ink a mixture of water, soot and Gum Arabic was in use. In the 19th century soot was very important for the rapidly developing rubber industry. With soot-filled shellac records it was possible to preserve sound recordings permanently. Since 1955 carbon fibers with highly ordered crystal structures were produced. Their use as reinforcement in polymer matrices opened the way of lightweight constructions, and particularly, they revolutionized the aircraft industries. Newly discovered nano-sized allotropisms of carbon, such as fullerenes, carbon nanotubes and finally graphene always seemed to be ideal materials to improve different polymers to adjust their properties for new needs. In addition to the homogeneous distribution of carbon-based particles, the filling and reinforcing of polymer matrices require a sufficient compatibility between the particle surfaces and the matrices. Particularly, surface modifications carried out on the particles appear well suited to improve the dispersibility and compatibility of the carbon-based fillers. However, a hindrance is a low reactivity due to the high chemical stability of graphite lattices and graphite-like structures. The degree of surface modification reactions is usually small, and the detection of newly formed functional surface groups is not trivial. In order to demonstrate the synthetic challenge of the surface modification of carboneous material different established concepts were briefly discussed. The focus of our work was directed to endow nano-sized carbon allotropes with primary amino groups, which are highly reactive to epoxy-carrying low-molecular weight substances or pre-polymers. For the surface modification we employed different natural and synthetic polyamines and a simple application of the polyamines from their aqueous solutions and in their processing at room temperature.