The preparation of the dicyano monomer precursor 2'-(2-(pyridin-4-yl)ethyl)-[1,1':4',1''terphenyl]-4,4''-dicarbonitrile, M3-py in Scheme 1, containing a dangling pyridine group used for the preparation of the triazine 2D polymer, involves a multistep organic synthesis using 2,5dibromotoluene as a starting material (See SI, Scheme S1). The reaction of M3-py with triflic acid in chloroform for 48 h at RT catalyzes its polymerization, generating a pale yellow powder of the corresponding covalent triazine framework (CTF) as shown in Scheme 1. The latter reacts with the Ru water oxidation catalyst precursor [Ru(tda)(dmso)(py)] (py is pyridine), in MeOH/EtOH (1:1) at reflux temperature for 3 days, producing a purple powder of the desired Ru-CTF hybrid molecular material, whose structure is drawn in Scheme 1. All the intermediates and precursors have been characterized by the usual analytic and spectroscopic techniques and are reported in the SI (Fig. ). The IR spectrum of the CTF material showed the absence of the νC≡N band at ca. 2220 cm -1 , which is indicative of a high degree of polymerization (Fig. ). Further, powder X-ray diffraction (PXRD) for both CTF and Ru-CTF shows a low degree of crystallinity, typical for this type of materials (Fig. ). Nitrogen absorption-desorption experiments reveal that CTF has a low surface area with SABET = 7.48 m 2 /g and low porosity (average pore diameter of 54 nm, associated to a non-uniform aggregation of particles) (Fig. ), supported by scanning electron microscopy (SEM) and transmission electron microscopy (TEM) techniques (Fig. and S9, respectively), which show disordered layers and agglomerated particles of different sizes.