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The structural, magnetic, and electron-transport properties of Heusler-ordered CoFeCrAl thin films are investigated experimentally and theoretically. The films, sputtered onto MgO and having thicknesses of about 100nm, exhibit virtually perfect single-crystalline epitaxy and a high degree of L21 chemical order. X-ray diffraction and transmission-electron microscopy show that the structure of the films is essentially of the L21 Heusler type. The films are ferrimagnetic, with a Curie temperature of about 390K, and a net moment of 2 μB per formula unit. The room temperature resistivity is 175 μΩ; the carrier concentration and mobility determined from the low temperature (5 K) measurement are 1.2 x 1018 cm-3 and 33 cm²/Vs, respectively. In contrast to the well-investigated Heusler alloys such as Co2(Cr1-xFex)Al, the CoFeCrAl system exhibits two main types of weak residual A2 disorder, namely, Co-Cr disorder and Fe-Cr disorder, the latter conserving half-metallicity. Point-contact Andreev reflection yields a lower bound for the spin polarization, 68% at 1.85K, but our structural and magnetization analyses suggest that the spin polarization at the Fermi level is probably higher than 90%. The high resistivity, spin polarization, and Curie temperature are encouraging in the context of spin electronics. [ABSTRACT FROM AUTHOR]