Accompanied　by　solid-state　structural　phase　transitions,　the　switchable　molecular　dynamics　(MD)　and　orderdisorder　transformation　of　(i-PrNHMe2)　thorn　cation　embedded　in　a　deformable　{[Ni(NCS)6]4-}&　INFIN;　supramolecular　framework　are　in-depth　investigated　by　variable-temperature　tests　of　single-crystal　X-ray　diffraction,　dielectric　measurement,　and　MD　simulation.　Interestingly,　it　is　found　that　the　confined　swinging　or　flipping　of　the　(iPrNHMe2)　thorn　cation　as　a　whole　is　assisted　by　a　synergistic　change　of　its　torsion　angle.　This　research　provides　a　helpful　insight　into　the　solid-state　MD　of　moderate-sized　quasi-spherical　molecules/ions　that　feature　a　flexible　inner　core.