In this study, we comprehensively investigated the growth of β-Ga 2 O 3 on (001) on-axis Ga 2 O 3 substrates via metalorganic chemical vapor deposition (MOCVD) using both triethylgallium (TEGa) and trimethylgallium (TMGa) as the Ga precursors. For MOCVD growth with TEGa, the group VI/III molar ratio was tuned with different TEGa molar flow rates. The correlation between growth conditions and the surface morphology, growth rate, and electron transport properties of MOCVDgrown (001) β-Ga 2 O 3 thin films is comprehensively analyzed. Room temperature mobility of 85 cm 2 /V s with carrier concentration of 2.0 × 10 17 cm −3 was measured for a film grown using the TEGa molar flow rate of 19 μmol/min and VI/III molar ratio of 934. For MOCVD growth of (001) Ga 2 O 3 using TMGa, we observed the occurrence of cracking along the [010] direction in the grown films, which was found to be closely related to the film thickness and growth rate. The relatively smooth surface morphology of the films with cracks is attributed to the strain relaxation. (001) β-Ga 2 O 3 films containing rotation domains with (−401) plane were observed from high-resolution X-ray diffraction (XRD) and confirmed with atomic-resolution scanning transmission electron microscopy (STEM) imaging. Under the same growth condition, (001) β-Ga 2 O 3 films contain higher carbon concentration as compared to that of the (010) β-Ga 2 O 3 films. Results from this work provide fundamental insights into the MOCVD epitaxy of β-Ga 2 O 3 on (001) Ga 2 O 3 substrates, revealing the opportunities and challenges of MOCVD growth of (001) β-Ga 2 O 3 thin films with fast growth rates for high-power electronic device technology.