We demonstrate precise control of the lower critical solution temperature (LCST) behavior of a thermoresponsive polymer in water by pillararene-based host-guest interactions. The LCST value of the polymer increases upon the stepwise addition of either of the two pillararene hosts. On account of the pH-responsiveness of the pillararene-based host-guest interactions, the recovery of the LCST is achieved by treatment with acid, reflecting the pH-responsive supramolecular control of the LCST.