  Magnetic transition metal dichalcogenide (TMD) films have recently emerged as
promising candidates to host novel magnetic phases relevant to next-generation
spintronic devices. However, systematic control of the magnetization
orientation, or anisotropy, and its thermal stability, characterized by Curie
temperature (Tc) remains to be achieved in such films. Here we present
self-intercalated epitaxial Cr1+{\delta}Te2 films as a platform for achieving
systematic/smooth magnetic tailoring in TMD films. Using a molecular beam
epitaxy (MBE) based technique, we have realized epitaxial Cr1+{\delta}Te2 films
with smoothly tunable over a wide range (0.33-0.82), while maintaining
NiAs-type crystal structure. With increasing {\delta}, we found monotonic
enhancement of Tc from 160 to 350 K, and the rotation of magnetic anisotropy
from out-of-plane to in-plane easy axis configuration for fixed film thickness.
Contributions from conventional dipolar and orbital moment terms are
insufficient to explain the observed evolution of magnetic behavior with
{\delta}. Instead, ab initio calculations suggest that the emergence of
antiferromagnetic interactions with {\delta}, and its interplay with
conventional ferromagnetism, may play a key role in the observed trends. To our
knowledge, this constitutes the first demonstration of tunable Tc and magnetic
anisotropy across room temperature in TMD films, and paves the way for
engineering novel magnetic phases for spintronic applications.
