Formation of nonequilibrium delta-Al5 Cr thin films prepared by sputter deposition has been studied. Among processing parameters examined, working pressure, deposition temperature, and time were found to play an important role in affecting the formation of delta-Al5 Cr phase. Susceptibility of delta-Al5 Cr formation to the processing condition was essentially ascribed to its metastable nature. Since it could irreversibly transform into the equilibrium alpha-BCC Cr upon heating, the nonequilibrium delta-Al5 Cr became unfavorable to form under the processing conditions that led to significant increases in film surface temperature such as lengthy depositions or elevated deposition temperatures. During the lengthy deposition, the film surface temperature inevitably increased as a result of continuous energetic particle bombardments. Such film surface temperature increase was analogous to an in situ annealing that was detrimental to the formation of thicker delta-Al5 Cr films. To minimize the in situ annealing effect, thr deposition with prolonged intermissions has showed very effectively to grow the relatively thick Cr films that had the nonequilibrium delta-Al5 crystal structure.