Magnetic 2D materials have emerged as a great interest in spintronics due to atomic thickness scaling, low energy switching, and ease in the manipulation of spins. This report demonstrates a facile, bottom‐up, chemical vapor deposition approach for non‐van der Waals (non‐vdWs), 2D chromium (III) sulfide (Cr2S3) with c‐axis orientation, out‐of‐plane magnetic anisotropy (easy axis), and ferrimagnetic ordering. Importantly, the anisotropic magnetic saturation and resistivity of 10.23 mΩ cm reveal a narrow bandgap ferrimagnetism in Cr2S3 (∆EActivation ≈ 22 meV and Eg ≈ 40 meV). The prototype lateral spin‐channel Al/Cr2S3/Al devices exhibit a negative magnetoresistance of ≈25% and ≈15% at 100 K (below Néel temperature) for few‐layer (≈8 nm) and thin‐film (≈50 nm) device structures, respectively, owing to itinerant ferrimagnetism of Cr2S3. The magnetic field‐induced spin polaron formations are quite resilient and enhance the field‐dependent carrier conduction, making it greatly useful for negative magnetoresistance operation. These prototype Al/Cr2S3/Al structures have demonstrated a low power (≈2 µW for 8 µm channel at 10 µA current) operation with a negative field‐dependent resistance coefficient (rM) of ≈−5 × 10−4 Oe−1. The computed rM magnitude is tenfold higher than the bulk Cr2S3. This study identifies the potential of non‐vdW Cr2S3 toward new and robust 2D‐based spintronic applications.