We observed a high compensation temperature (T-comp) of 175 K in a vanadium hexacyanochromate-based ferrimagnet, KI0.19 V-0.64(II) (V-IV O)(0.36)[Cr-III(CN)(6)](0.73)center dot 7.5H(2)O. The observed phenomenon is understood by the compensation of the positive sublattice magnetization of Cr-III (S = 3/2) and the negative sublattice magnetizations of V-II (S = 3/2) and V-IV (S = 1/2). A T-comp value of 175 K is the highest value among moleculebased magnets reported to date.