Actinyl oxysalts with TO4 tetrahedral oxyanions (T = S, Se, Cr, Mo) demonstrate a remarkable structural diversity, owing to the flexibility of the An–O–T linkages, which results in a multitude of topological and geometrical variations. Application of graph representation of structural units allows topological classification of structures and analysis of topological and geometrical isomers. In some organically templated structures, isomerism is controlled by the interplay of hydrophobic/hydrophilic interactions between organic and inorganic substructures. The high flexibility of actinyl oxysalt complexes (in particular, in uranyl selenates) allows strong curvature of inorganic units and formation of curved nanoscale tubules assembled from [1+4+1] complexes. In some particular systems, the self‐assembly process may be modeled using a cellular automata approach.