An excellent molecule‐based cryogenic magnetic refrigerant, gadolinium acetate tetrahydrate, is here used to decorate selected portions of silicon substrate. By quantitative magnetic force microscopy for a variable applied magnetic field near liquid‐helium temperature, the molecules are demonstrated to hold their magnetic properties intact, and therefore their cooling functionality, after their deposition. These results represent a step forward towards the realization of a molecule‐based micro‐refrigerating device at very low temperatures.