The fabrication of smart, efficient, and innovative devices critically needs highly refined thin‐film nanomaterials; therefore, facile, scalable, and economical methods of thin films production are highly sought‐after for the sustainable growth of the hi‐tech industry. The chemical vapor deposition (CVD) technique is widely implemented at the industrial level due to its versatile features. However, common issues with a precursor, such as reduced volatility and thermal stability, restrict the use of CVD to produce novel and unique materials. A modified CVD approach, named aerosol‐assisted CVD (AACVD), has been the center of attention due to its remarkable tendency to fabricate uniform, homogenous, and distinct nano‐architecture thin films in an uncomplicated and straightforward manner. Above all, AACVD can utilize any custom‐made or commercially available precursors, which can be transformed into a transparent solution in a common organic solvent; thus, a vast array of compounds can be used for the formation of nanomaterial thin films. This review article highlights the importance of AACVD in fabricating heterobimetallic oxide thin films and their potential in making energy production (e. g., photoelectrochemical water splitting), energy storage (e. g., supercapacitors), and environmental protection (e. g., electrochemical sensors) devices. A heterobimetallic oxide system involves two metallic species either in a composite, solid solution, or metal‐doped metal oxides. Moreover, the AACVD tunable parameters, such as temperature, deposition time, and precursor, which drastically affect thin films microstructure and their performance in device applications, are also discussed. Lastly, the key challenges and issues of scaling up AACVD to the industrial level and processing for emerging functional materials are also highlighted.