Recently, a new calcium-ferrite-type Cr oxide, NaCr 2 O 4 , was synthesized by high-pressure synthesis, and was found to show unconventional colossal magnetoresistance (CMR) effect below the canted-antiferromagnetic (AF) transition temperature of T N = 125 K. The CMR effect becomes more prominent with decreasing temperature, and the magnetoresistance at each temperature shows a significant change with no field hysteresis within the canted-AF phase, which warrants the unconventional nature of the CMR. Magnetic susceptibility of the compound clearly indicates that the magnetic transition is AF, not ferromagnetic, although spontaneous magnetization appears below T N . Above spin-flop transition field, magnetic susceptibility shows unusual behavior.