  Nanoscale layered ferromagnets have demonstrated fascinating two-dimensional
magnetism down to atomic layers, providing a peculiar playground of spin orders
for investigating fundamental physics and spintronic applications. However,
strategy for growing films with designed magnetic properties is not well
established yet. Herein, we present a versatile method to control the Curie
temperature (T_{C}) and magnetic anisotropy during growth of ultrathin
Cr_{2}Te_{3} films. We demonstrate increase of the TC from 165 K to 310 K in
sync with magnetic anisotropy switching from an out-of-plane orientation to an
in-plane one, respectively, via controlling the Te source flux during film
growth, leading to different c-lattice parameters while preserving the
stoichiometries and thicknesses of the films. We attributed this modulation of
magnetic anisotropy to the switching of the orbital magnetic moment, using
X-ray magnetic circular dichroism analysis. We also inferred that different
c-lattice constants might be responsible for the magnetic anisotropy change,
supported by theoretical calculations. These findings emphasize the potential
of ultrathin Cr_{2}Te_{3} films as candidates for developing room-temperature
spintronics applications and similar growth strategies could be applicable to
fabricate other nanoscale layered magnetic compounds.
