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Here, through experimental and simulation studies, we prove the role of co-ions as a function of co-ion size to their interaction aided by the macroions (using and as designs) therefore the associated self-assembly into blackberry-type structures in dilute solutions. A few regimes of special co-ion impacts tend to be clearly identified little ions (halides, oxoacid ions), subnanometer-scaled large ions (lacunary Keggin and dodecaborate ions), and the ones with sizes much like t