The oriented growth of β‐Ga2O3 films has triggered extensive interest due to the remarkable and complex anisotropy found in the β‐Ga2O3 bulks. Remarkable properties, including stronger solar‐blind ultraviolet (SBUV) absorption, better mobility, and higher thermal conductivity, are usually observed along <010> direction as compared to other low‐index axes. So far, <010>‐oriented β‐Ga2O3 film growth has been hindered by the lack of suitable substrates and higher surface energy of the (010) crystal plane. Herein, the first growth of uniquely <010>‐oriented β‐Ga2O3 films on quartz substrates by laser chemical vapor deposition (LCVD) are reported. By investigating the effects of deposition temperature (Tdep) and O2 flow rate (RO2) on the growth of β‐Ga2O3 films, it is found that the formation of <010> orientation is closely related to the higher stability of oxygen close‐packed planes under O‐rich condition. As a result, a grain size of up to ≈2 µm and a deposition rate of up to ≈ 40 µm h−1 are obtained. Metal‐semiconductor‐metal (MSM) type detector based on <010>‐oriented β‐Ga2O3 film exhibits ultra‐fast response speed, 1–2 orders of magnitude higher than those of most detectors based on β‐Ga2O3 films with other orientations.