To obtain a high field emission (FE) current with a low driving voltage, it is important to control and optimize carbon nanofiber (CNF) array patterns for FE. While there have been various means for controlling CNF array patterns reported over the past few decades, array patterning using lithography is the method typically used to control CNF morphology. Because lithography uses many masks and is costly, it is necessary to establish a simpler process. In this study, the grain size and distribution of catalysts with phase separation were controlled. A system which controls the morphology of small bundles of CNFs was constructed with the distance between the bundles kept constant in order to obtain a higher FE current. The Ni catalyst layer for forming the CNF morphology was separated by noncatalytic Cr grains formed by cosputtering. As a result, it was possible to control the Ni content, the grain size and synthesis density of CNFs in the alloy with a varying number of nickel pellets placed on the chromium target. This method is an epochmaking CNF patterning technique very different from lithography.