Radical templation centered around a heterotrisradical tricationic inclusion complex DB center dot+subset of DAPQT2((center dot+)), assembled from an equimolar mixture of a disubstituted 4,4'-bipyridinium radical cation (DB center dot+) and an asymmetric cyclophane bisradical dication DAPQT2((center dot+))), affords a symmetric [2]catenane (SC center dot 7PF(6)) and an asymmetric [2]catenane (AC center dot 7PF(6)) on reaction of the 1:1 complex with diazapyrene and bipyridine, respectively. Both these highly charged [2]catenanes have been isolated as air-stable monoradicals and characterized by EPR spectroscopy. X-ray crystallography suggests that the unpaired electrons are delocalized in each case across two inner 4,4'-bipyridinium (BIPY2+) units forming a mixed-valence (BIPY2)(center dot 3+) state inside both [2]catenanes, an observation which is in good agreement with spin-density calculations using density functional theory. Electrochemical studies indicate that by replacing the BIPY2+ units in homo[2]catenane HC center dot 7+-composed of two mechanically interlocked cyclobis(paraquat-p-phenylene) rings-with zero, one, and two more highly conjugated diazapyrenium dication (DAP(2+)) units, respectively, a consecutive series of five, six, and seven redox states can be accessed in the resulting SC center dot 7PF(6) (0, 4+, 6+, 7+, and 8+), HC center dot 7PF(6) (0, 2+, 4+, 6+, 7+, and 8+), and AC center dot 7PF(6) (0, 1+, 2+, 4+, 6+, 7+, and 8+), respectively. These unique [2]catenanes present a promising prototype for the fabrication of high-density data memories.