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To design and synthesize high‐nucleated titanium‐oxo clusters rationally based on molecular building blocks with potential coordination ability is still a great challenge. In this work, a family of titanium‐oxo clusters, including Ti2, Ti6, Ti12, and Ti20 clusters, have been assembled from large‐size ligand embonic acid‐modified {Ti2} molecular building blocks under solvothermal conditions. By modulating...