Three new high-dimensional cucurbit[6]-based metal–organic rotaxane frameworks [Co₂(PR43)(BDC)₂Cl₂]·4H₂O (1), [Co₂(PR43)(BTC)₂]·6H₂O (2) and [Co₂(PR43)(BPT)₂]·20H₂O (3) were obtained via the hydrothermal synthesis method. Compound 1 comprised a two-dimensional layered structure, while compounds 2 and 3 exhibited three-dimensional pillared structures. All the compounds showed good thermal stabilities. Furthermore, the magnetic properties of compounds 1–3 were also investigated in detail.