Atomic intercalation can be utilized to engineer the electronic structure of two dimensional layered materials at the atomic scale, thereby governing distinctive properties in comparison with the pristine ones. Herein, a minute amount of Rhenium (Re) atoms (∼1.3% wt.) were controllably intercalated inside the layers of semiconducting Zirconium diselenide (ZrSe2) single crystal. Our angle-resolved photoemission spectroscopy revealed that Re intercalation could move down the bottom of the ZrSe2 conduction band without band dispersion changes, resulting in a small electronic pocket at the Brillouin zone boundary at the M point. The subsequent low-temperature transport results further confirmed the anomalous metallic characteristics in the semiconducting ZrSe2 after low-level Re intercalation.