An experimental study is presented of the rotational magnetocaloric effect in a KTm(MoO4)2 single crystal at temperatures above 2 K associated with the rotation of a single crystal between the magnetic easy and hard axis in constant magnetic fields up to 5 T. The magnetocaloric properties of KTm(MoO4)2 single crystals are investigated by isothermal magnetization measurements. The maximal rotational entropy change −ΔSR ≈ 9.8 J/(kgK) is achieved at 10 K in a magnetic field of 5 T. The adiabatic rotation of a single crystal in a field of 5 T at an initial temperature of 4.2 K causes cooling of the sample down to 0.5 K, which indicates an interesting possibility of using this material for cooling processes at low temperatures.