The chemistry of polypyridyl Ru(II) and cyclometalated Ir(III) derivatives provides long-lasting interest to researchers due to the inherent advantage of their triplet states in a variety of photoactivities. The introduction of Ru(N^N)3 and Ir(C^N)2(X^N) modules into well-defined architectures extends the research areas of both photoactive metal complexes and network chemistry, generating a lot of new opportunities with interesting structural aesthetics and profound functional possibilities. The rapid development of research in integrating Ru(II) or Ir(III) metallotecons into the architectures has been apparent in recent years which makes this a fascinating subject for reviewing. This review focuses on the design and syntheses of Ru(N^N)3 and Ir(C^N)2(X^N) functionalized architectures of metal-organic frameworks (MOFs), covalent-organic frameworks (COFs), metallasupramolecules, organic supramolecules and supramolecular organic frameworks (SOFs). Furthermore, the photocatalytic applications including the hydrogen evolution reaction (HER), carbon dioxide reduction reaction (CO2RR), photocatalytic oxidation and photoredox catalysis of organic transformation are also presented.