Covalent triazine frameworks (CTFs) represent a new type of porous organic material, obtained through the formation of triazine units that act as covalent linkage along the porous structure of the system. CTFs have some unique physical and chemical properties, i.e., large surface area, permanent porosity, rich nitrogen content, heterocyclic nuclei, and absence of any weak bonds. The strong aromatic covalent bonds endow CTFs with high chemical and thermal stability. These remarkable features make CTFs promising materials for a wide range of applications, including heterogeneous catalysis. In particular, the use of these materials as catalytic supports for metal nanoparticles represents a very interesting and intensely investigated research field. Given the current interest, this thesis aims to obtain CTF materials through different synthetic strategies, on which nickel nanoparticles will be deposited. This latter task will be pursued by the metal vapor synthesis (MVS) approach, as well as by the use of organometallic nickel precursors. After having investigated the morphological and structural features of the heterogeneous Ni catalysts thus obtained, their ability to promote the hydrolysis of ammonia borane and the transfer hydrogenation reactions of different unsaturated compounds, using ammonia borane, will be studied. The catalytic properties of CTFs-supported Ni nanoparticles will also be compared with that of commercial carbon-supported Ni NPs, prepared by the same way.