Amorphous coordination nanoparticles (CNPs) formed from metal ions and synthetic ligand molecules have been emerging as a new family of functional nanomaterials. [1] They are made up of polymeric networks of ligands and metal ions [2] and have been applied in many fields including catalysis, [3] bioimaging [4] and drug delivery. [5] The majority of CNPs reported to date contain hydrophobic ligand molecules and consequently they have mostly been prepared in organic media. Meanwhile, we have recently reported that water-soluble nucleotides serve as bidentate ligands. [6] Upon mixing nucleotides and lanthanide ions in water, coordination networks consisting of phosphate, nucleobase units and lanthanide ions form spontaneously and give amorphous nanoparticle structures as determined by X-ray diffraction analysis. [6b] These nucleotide/lanthanide CNPs enjoy the full benefits of using biomolecules and lanthanide ions in water. For example, the large coordination number of lanthanide ions allows formation of amorphous coordination networks, in which densely accumulated nucleotides and lanthanide ions reveal efficient energy transfer and remarkable magnetic resonance imaging (MRI) properties. [6b] Moreover, they exhibit surprisingly adaptive self-assembly properties, that is, amorphous coordination networks are formed around a variety of water-soluble guest materials during the course of assembly. [6b,c] The design of adaptive self assembly is considered to be one of the forthcoming issues in supramolecular chemistry. [7] We herein report a novel approach to bring out the latent photofunctionality of nucleotide/lanthanide complexes by inclusion of guest cofactor molecules. Synergistic interactions that operate between the cofactor ligands and host coordination networks confer the nucleotide/lanthanide CNPs