We report the magnetovolume effect of quaternary Heusler alloy CoFeCrAl as a potential candidate of spin gapless semiconductor. The crystal structure of CoFeCrAl was confirmed as the single phase of the ordered LiMgPdSn-type structure. From magnetization measurements at ambient pressure, the Curie temperature TC and the spontaneous magnetization Ms were determined to be 575.2 K and 2.01 μ B/f.u., respectively. The TC is higher enough than room temperature and the Ms follows the Slater-Pauling rule. High-pressure magnetization measurements showed that the Ms is almost independent of applying pressures not only at 10 K but also up to 300 K, exhibiting that the electronic state of CoFeCrAl is fully spin polarized and it is preserved even at 300 K. The experimental results reveal that the quaternary Heusler alloy CoFeCrAl is an attractive material for functional electrode ferromagnets in spintronics devices.